Directional Forces by Momentumless Excitation and Order-to-Order Transition in Peierls-Distorted Solids: The Case of GeTe

NASA Astrophysics Data System (ADS)

Chen, Nian-Ke; Li, Xian-Bin; Bang, Junhyeok; Wang, Xue-Peng; Han, Dong; West, Damien; Zhang, Shangbai; Sun, Hong-Bo

2018-05-01

Time-dependent density-functional theory molecular dynamics reveals an unexpected effect of optical excitation in the experimentally observed rhombohedral-to-cubic transition of GeTe. The excitation induces coherent forces along [001], which may be attributed to the unique energy landscape of Peierls-distorted solids. The forces drive the A1 g optical phonon mode in which Ge and Te move out of phase. Upon damping of the A1 g mode, phase transition takes place, which involves no atomic diffusion, defect formation, or the nucleation and growth of the cubic phase.

A small animal time-resolved optical tomography platform using wide-field excitation

NASA Astrophysics Data System (ADS)

Venugopal, Vivek

Small animal imaging plays a critical role in present day biomedical research by filling an important gap in the translation of research from the bench to the bedside. Optical techniques constitute an emerging imaging modality which have tremendous potential in preclinical applications. Optical imaging methods are capable of non-invasive assessment of the functional and molecular characteristics of biological tissue. The three-dimensional optical imaging technique, referred to as diffuse optical tomography, provides an approach for the whole-body imaging of small animal models and can provide volumetric maps of tissue functional parameters (e.g. blood volume, oxygen saturation etc.) and/or provide 3D localization and quantification of fluorescence-based molecular markers in vivo. However, the complex mathematical reconstruction problem associated with optical tomography and the cumbersome instrumental designs limits its adoption as a high-throughput quantitative whole-body imaging modality in current biomedical research. The development of new optical imaging paradigms is thus necessary for a wide-acceptance of this new technology. In this thesis, the design, development, characterization and optimization of a small animal optical tomography system is discussed. Specifically, the platform combines a highly sensitive time-resolved imaging paradigm with multi-spectral excitation capability and CCD-based detection to provide a system capable of generating spatially, spectrally and temporally dense measurement datasets. The acquisition of such data sets however can take long and translate to often unrealistic acquisition times when using the classical point source based excitation scheme. The novel approach in the design of this platform is the adoption of a wide-field excitation scheme which employs extended excitation sources and in the process allows an estimated ten-fold reduction in the acquisition time. The work described herein details the design of the imaging platform employing DLP-based excitation and time-gated intensified CCD detection and the optimal system operation parameters are determined. The feasibility this imaging approach and accuracy of the system in reconstructing functional parameters and fluorescence markers based on lifetime contrast is established through phantom studies. As a part of the system characterization, the effect of noise in time-resolved optical tomography is investigated and propagation of system noise in optical reconstructions is established. Furthermore, data processing and measurement calibration techniques aimed at reducing the effect of noise in reconstructions are defined. The optimization of excitation pattern selection is established through a novel measurement-guided iterative pattern correction scheme. This technique referred to as Adaptive Full-Field Optical Tomography was shown to improve reconstruction performances in murine models by reducing the dynamic range in photon flux measurements on the surface. Lastly, the application of the unique attributes of this platform to a biologically relevant imaging application, referred to as Forster Resonance Energy Transfer is described. The tomographic imaging of FRET interaction in vivo on a whole-body scale is achieved using the wide-field imaging approach based on lifetime contrast. This technique represents the first demonstration of tomographic FRET imaging in small animals and has significant potential in the development of optical imaging techniques in varied applications ranging from drug discovery to in vivo study of protein-protein interaction.

Dynamic nano-imaging of label-free living cells using electron beam excitation-assisted optical microscope

PubMed Central

Fukuta, Masahiro; Kanamori, Satoshi; Furukawa, Taichi; Nawa, Yasunori; Inami, Wataru; Lin, Sheng; Kawata, Yoshimasa; Terakawa, Susumu

2015-01-01

Optical microscopes are effective tools for cellular function analysis because biological cells can be observed non-destructively and non-invasively in the living state in either water or atmosphere condition. Label-free optical imaging technique such as phase-contrast microscopy has been analysed many cellular functions, and it is essential technology for bioscience field. However, the diffraction limit of light makes it is difficult to image nano-structures in a label-free living cell, for example the endoplasmic reticulum, the Golgi body and the localization of proteins. Here we demonstrate the dynamic imaging of a label-free cell with high spatial resolution by using an electron beam excitation-assisted optical (EXA) microscope. We observed the dynamic movement of the nucleus and nano-scale granules in living cells with better than 100 nm spatial resolution and a signal-to-noise ratio (SNR) around 10. Our results contribute to the development of cellular function analysis and open up new bioscience applications. PMID:26525841

Dynamic nano-imaging of label-free living cells using electron beam excitation-assisted optical microscope.

PubMed

Fukuta, Masahiro; Kanamori, Satoshi; Furukawa, Taichi; Nawa, Yasunori; Inami, Wataru; Lin, Sheng; Kawata, Yoshimasa; Terakawa, Susumu

2015-11-03

Optical microscopes are effective tools for cellular function analysis because biological cells can be observed non-destructively and non-invasively in the living state in either water or atmosphere condition. Label-free optical imaging technique such as phase-contrast microscopy has been analysed many cellular functions, and it is essential technology for bioscience field. However, the diffraction limit of light makes it is difficult to image nano-structures in a label-free living cell, for example the endoplasmic reticulum, the Golgi body and the localization of proteins. Here we demonstrate the dynamic imaging of a label-free cell with high spatial resolution by using an electron beam excitation-assisted optical (EXA) microscope. We observed the dynamic movement of the nucleus and nano-scale granules in living cells with better than 100 nm spatial resolution and a signal-to-noise ratio (SNR) around 10. Our results contribute to the development of cellular function analysis and open up new bioscience applications.

Dynamic nano-imaging of label-free living cells using electron beam excitation-assisted optical microscope

NASA Astrophysics Data System (ADS)

Fukuta, Masahiro; Kanamori, Satoshi; Furukawa, Taichi; Nawa, Yasunori; Inami, Wataru; Lin, Sheng; Kawata, Yoshimasa; Terakawa, Susumu

2015-11-01

Optical microscopes are effective tools for cellular function analysis because biological cells can be observed non-destructively and non-invasively in the living state in either water or atmosphere condition. Label-free optical imaging technique such as phase-contrast microscopy has been analysed many cellular functions, and it is essential technology for bioscience field. However, the diffraction limit of light makes it is difficult to image nano-structures in a label-free living cell, for example the endoplasmic reticulum, the Golgi body and the localization of proteins. Here we demonstrate the dynamic imaging of a label-free cell with high spatial resolution by using an electron beam excitation-assisted optical (EXA) microscope. We observed the dynamic movement of the nucleus and nano-scale granules in living cells with better than 100 nm spatial resolution and a signal-to-noise ratio (SNR) around 10. Our results contribute to the development of cellular function analysis and open up new bioscience applications.

Images of photoreceptors in living primate eyes using adaptive optics two-photon ophthalmoscopy

PubMed Central

Hunter, Jennifer J.; Masella, Benjamin; Dubra, Alfredo; Sharma, Robin; Yin, Lu; Merigan, William H.; Palczewska, Grazyna; Palczewski, Krzysztof; Williams, David R.

2011-01-01

In vivo two-photon imaging through the pupil of the primate eye has the potential to become a useful tool for functional imaging of the retina. Two-photon excited fluorescence images of the macaque cone mosaic were obtained using a fluorescence adaptive optics scanning laser ophthalmoscope, overcoming the challenges of a low numerical aperture, imperfect optics of the eye, high required light levels, and eye motion. Although the specific fluorophores are as yet unknown, strong in vivo intrinsic fluorescence allowed images of the cone mosaic. Imaging intact ex vivo retina revealed that the strongest two-photon excited fluorescence signal comes from the cone inner segments. The fluorescence response increased following light stimulation, which could provide a functional measure of the effects of light on photoreceptors. PMID:21326644

Nano-optical functionality based on local photoisomerization in photochromic single crystal

NASA Astrophysics Data System (ADS)

Nakagomi, Ryo; Uchiyama, Kazuharu; Kubota, Satoru; Hatano, Eri; Uchida, Kingo; Naruse, Makoto; Hori, Hirokazu

2018-01-01

Towards the construction of functional devices and systems using optical near-field processes, we demonstrate the multivalent features in the path-branching phenomena in a photochromic single crystal observed in optical phase change between colorless (1o) and blue-colored (1c) phases that transmits in subwavelength scale over a macroscopic spatial range associated with local mechanical distortions induced. To observe the near-field optical processes of transmission path branching, we have developed a top-to-bottom double-probe scanning near-field optical microscope capable of nanometer-scale correlation measurements by two individually position-controlled probes that face each other sandwiching the photochromic material. We have experimentally confirmed that a local near-field optical excitation applied to one side of the photochromic crystal by a probe tip resulted in characteristic structures of subwavelength scale around 100 nm or less that are observed by the other probe tip located on the opposite side. The structures are different from those resulting from far-field excitations that are quantitively evaluated by autocorrelations. The results suggest that the mechanical distortion caused by the local phase change in the photochromic crystal suppresses the phase change of the neighboring molecules. This new type of optical-near-field-induced local photoisomerization has the potential to allow the construction of functional devices with multivalent properties for natural intelligence.

A novel low cost pulse excitation source to study trap spectroscopy of persistent luminescent materials

NASA Astrophysics Data System (ADS)

Chandrasekhar, Ngangbam; Singh, Nungleppam Monorajan; Gartia, R. K.

2018-04-01

Luminescent techniques require one or the other source of excitations which may vary from high cost X-rays, γ-rays, β-rays etc. to low cost LED. Persistent luminescent materials or Glow-in-the-Dark phosphors are the optical harvesters which store the optical energy from day light illuminating a whole night. They are so sensitive that they can be excited even with the low light of firefly. Therefore, instead of using a high cost excitation source authors have developed a low cost functioning of excitation source controlling short pulses of LED to excite persistent phosphors with the aid of ExpEYES Junior (Hardware/software framework developed by IUAC, New Delhi). Using this, the authors have excited the sample under investigation upto 10 ms. Trap spectroscopy of the pre-excited sample with LED is studied using Thermoluminescence (TL) technique. In this communication, development of the excitation source is discussed and demonstrate the its usefulness in the study of trap spectroscopy of commercially available CaS:Eu2+, Sm3+. Trapping parameters are also evaluated using Computerized Glow Curve Deconvolution (CGCD) technique.

A systematic benchmark of the ab initio Bethe-Salpeter equation approach for low-lying optical excitations of small organic molecules

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

Bruneval, Fabien; Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720; Department of Physics, University of California, Berkeley, California 94720

2015-06-28

The predictive power of the ab initio Bethe-Salpeter equation (BSE) approach, rigorously based on many-body Green’s function theory but incorporating information from density functional theory, has already been demonstrated for the optical gaps and spectra of solid-state systems. Interest in photoactive hybrid organic/inorganic systems has recently increased and so has the use of the BSE for computing neutral excitations of organic molecules. However, no systematic benchmarks of the BSE for neutral electronic excitations of organic molecules exist. Here, we study the performance of the BSE for the 28 small molecules in Thiel’s widely used time-dependent density functional theory benchmark setmore » [Schreiber et al., J. Chem. Phys. 128, 134110 (2008)]. We observe that the BSE produces results that depend critically on the mean-field starting point employed in the perturbative approach. We find that this starting point dependence is mainly introduced through the quasiparticle energies obtained at the intermediate GW step and that with a judicious choice of starting mean-field, singlet excitation energies obtained from BSE are in excellent quantitative agreement with higher-level wavefunction methods. The quality of the triplet excitations is slightly less satisfactory.« less

Final Technical Report [Scalable methods for electronic excitations and optical responses of nanostructures: mathematics to algorithms to observables

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

Saad, Yousef

2014-03-19

The master project under which this work is funded had as its main objective to develop computational methods for modeling electronic excited-state and optical properties of various nanostructures. The specific goals of the computer science group were primarily to develop effective numerical algorithms in Density Functional Theory (DFT) and Time Dependent Density Functional Theory (TDDFT). There were essentially four distinct stated objectives. The first objective was to study and develop effective numerical algorithms for solving large eigenvalue problems such as those that arise in Density Functional Theory (DFT) methods. The second objective was to explore so-called linear scaling methods ormore » Methods that avoid diagonalization. The third was to develop effective approaches for Time-Dependent DFT (TDDFT). Our fourth and final objective was to examine effective solution strategies for other problems in electronic excitations, such as the GW/Bethe-Salpeter method, and quantum transport problems.« less

Functional emergence of a column-like architecture in layer 5 of mouse somatosensory cortex in vivo.

PubMed

Koizumi, Kyo; Inoue, Masatoshi; Chowdhury, Srikanta; Bito, Haruhiko; Yamanaka, Akihiro; Ishizuka, Toru; Yawo, Hiromu

2018-05-14

To investigate how the functional architecture is organized in layer 5 (L5) of the somatosensory cortex of a mouse in vivo, the input-output relationship was investigated using an all-optical approach. The neural activity in L5 was optically recorded using a Ca 2+ sensor, R-CaMP2, through a microprism inserted in the cortex under two-photon microscopy, while the L5 was regionally excited using optogenetics. The excitability was spread around the blue-light irradiated region, but the horizontal propagation was limited to within a certain distance (λ < 130 μm from the center of the illumination spot). When two regions were photostimulated with a short interval, the excitability of each cluster was reduced. Therefore, a column-like architecture had functionally emerged with reciprocal inhibition through a minimal number of synaptic relays. This could generate a synchronous output from a region of L5 with simultaneous enhancement of the signal-to-noise ratio by silencing of the neighboring regions.

Numerical Green's functions in optical potential calculations for positron scattering from argon and neon

NASA Technical Reports Server (NTRS)

Bartschat, K.; Mceachran, R. P.; Stauffer, A. D.

1990-01-01

An optical potential method was applied to the calculation of positron scattering from the noble gases in order to determine the effect of open excitation channels on the shape of differential scattering cross sections.

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.

Digitally synthesized beat frequency-multiplexed fluorescence lifetime spectroscopy

PubMed Central

Chan, Jacky C. K.; Diebold, Eric D.; Buckley, Brandon W.; Mao, Sien; Akbari, Najva; Jalali, Bahram

2014-01-01

Frequency domain fluorescence lifetime imaging is a powerful technique that enables the observation of subtle changes in the molecular environment of a fluorescent probe. This technique works by measuring the phase delay between the optical emission and excitation of fluorophores as a function of modulation frequency. However, high-resolution measurements are time consuming, as the excitation modulation frequency must be swept, and faster low-resolution measurements at a single frequency are prone to large errors. Here, we present a low cost optical system for applications in real-time confocal lifetime imaging, which measures the phase vs. frequency spectrum without sweeping. Deemed Lifetime Imaging using Frequency-multiplexed Excitation (LIFE), this technique uses a digitally-synthesized radio frequency comb to drive an acousto-optic deflector, operated in a cat’s-eye configuration, to produce a single laser excitation beam modulated at multiple beat frequencies. We demonstrate simultaneous fluorescence lifetime measurements at 10 frequencies over a bandwidth of 48 MHz, enabling high speed frequency domain lifetime analysis of single- and multi-component sample mixtures. PMID:25574449

Efficient Predictions of Excited State for Nanomaterials Using Aces 3 and 4

DTIC Science & Technology

2017-12-20

by first-principle methods in the software package ACES by using large parallel computers, growing tothe exascale. 15. SUBJECT TERMS Computer...modeling, excited states, optical properties, structure, stability, activation barriers first principle methods , parallel computing 16. SECURITY...2 Progress with new density functional methods

Optical Excitation of Carbon Nanotubes Drives Localized Diazonium Reactions

PubMed Central

2016-01-01

Covalent chemistries have been widely used to modify carbon nanomaterials; however, they typically lack the precision and efficiency required to directly engineer their optical and electronic properties. Here, we show, for the first time, that visible light which is tuned into resonance with carbon nanotubes can be used to drive their functionalization by aryldiazonium salts. The optical excitation accelerates the reaction rate 154-fold (±13) and makes it possible to significantly improve the efficiency of covalent bonding to the sp2 carbon lattice. Control experiments suggest that the reaction is dominated by a localized photothermal effect. This light-driven reaction paves the way for precise nanochemistry that can directly tailor carbon nanomaterials at the optical and electronic levels. PMID:27588432

Peculiarities of Forming a Multiband Transmission Function Based on Multifrequency Acousto-Optic Diffraction

NASA Astrophysics Data System (ADS)

Proklov, V. V.; Rezvov, Yu. G.

2018-01-01

An analytical solution for the transmission function of noncoherent wideband radiation is obtained under acousto-optic (AO) filtering using a discrete set of monochromatic AO waves with a small spectral overlap. We studied characteristics of the AO transformation of a continuous spectrum of noncoherent radiation into a given set of discrete narrow bands of spectral transmission by excitation of a discrete set of sound frequencies. We carried out the analysis of transmission functions of individual channels taking into account a partial overlap of their spectra and possible intermodulation distortions. It is shown that a stationary value of the root-mean-square light power is found at the electronic output due to the photoelectric transformation and detecting diffracted light. Based on this, a necessary stationary, multiband, and nearly equidistant transmission function of a device can be formed by using a relevant spectrum of acoustic excitation. Peculiarities of this way of forming the multiband transmission function are revealed: the limitation of diffraction efficiency for an individual channel, the possibility of decoupling side lobes of adjacent channels, etc. A multiband acousto-optic filter (MAOF) was simulated that was based on a paratellurite monocrystal (TeO2), which was previously used for experimental optical encoding. The theoretical and experimental results are in gratifying agreement.

Optical properties of body-centered tetragonal C4: Insights from many-body perturbation and time-dependent density functional theories

NASA Astrophysics Data System (ADS)

Tarighi Ahmadpour, Mahdi; Rostamnejadi, Ali; Hashemifar, S. Javad

2018-04-01

We study the electronic structure and optical properties of a body-centered tetragonal phase of carbon (bct-C4) within the framework of time-dependent density functional theory and Bethe-Salpeter equation. The results indicate that the optical properties of bct-C4 are strongly affected by the electron-hole interaction. It is demonstrated that the long-range corrected exchange-correlation kernels could fairly reproduce the Bethe-Salpeter equation results. The effective carrier number reveals that at energies above 30 eV, the excitonic effects are not dominant any more and that the optical transitions originate mainly from electronic excitations. The emerged peaks in the calculated electron energy loss spectra are discussed in terms of plasmon excitations and interband transitions. The results of the research indicate that bct-C4 is an indirect wide-band-gap semiconductor, which is transparent in the visible region and opaque in the ultraviolet spectral range.

Group-Velocity-Controlled and Gate-Tunable Directional Excitation of Polaritons in Graphene-Boron Nitride Heterostructures

NASA Astrophysics Data System (ADS)

Jiang, Yuyu; Lin, Xiao; Low, Tony; Zhang, Baile; Chen, Hongsheng

2018-05-01

A fundamental building block in nano-photonics is the ability to directionally excite highly squeezed optical mode dynamically, particularly with an electrical bias. Such capabilities would enable the active manipulation of light propagation for information processing and transfer. However, when the optical source is built-in, it remains challenging to steer the excitation directionality in a flexible way. Here, we reveal a novel mechanism for tunable directional excitation of highly squeezed polaritons in graphene-hexagonal boron nitride (hBN) heterostructures. The effect relies on controlling the sign of the group velocity of the coupled plasmon-phonon polaritons, which can be flipped by simply tuning the chemical potential of graphene (through electrostatic gating) in the heterostructures. Graphene-hBN heterostructure thus present a promising platform toward nano-photonic circuits and nano-devices with electrically reconfigurable functionalities.

Electronic excitations in γ -Li2IrO3

NASA Astrophysics Data System (ADS)

Li, Ying; Winter, Stephen M.; Jeschke, Harald O.; Valentí, Roser

2017-01-01

We investigate the electronic properties of the three-dimensional stripyhoneycomb γ -Li2IrO3 via relativistic density functional theory calculations as well as exact diagonalization of finite clusters and explore the details of the optical conductivity. Our analysis of this quantity reveals the microscopic origin of the experimentally observed (i) optical transitions and (ii) anisotropic behavior along the various polarization directions. In particular, we find that the optical excitations are overall dominated by transitions between jeff=1 /2 and 3/2 states and the weight of transitions between jeff=1 /2 states at low frequencies can be correlated to deviations from a pure Kitaev description. We furthermore reanalyze within this approach the electronic excitations in the known two-dimensional honeycomb systems α -Li2IrO3 and Na2IrO3 and discuss the results in comparison to γ -Li2IrO3 .

Nonlinear reflection and refraction of ultrashort light pulses at the surfaces of resonant media and phase memory effects

NASA Astrophysics Data System (ADS)

Vlasov, R. A.; Gadomskii, O. H.; Gadomskaia, I. V.; Samartsev, V. V.

1986-06-01

The method of integrodifferential equations related to the optical Bloch equations is used to study the nonlinear reflection (or refraction) of a scanning laser beam at the surface of a resonant medium excited by traveling and standing surface electromagnetic waves at resonant frequency. The effect of the phase memory of surface atoms on the pulsed action of fields with space-time resolution is taken into account. The reversal of the scanning beam from the excited surface with phase conjugation of the wave front is considered. In addition, the spectrum of the nonlinear surface polaritons is analyzed as a function of the area of the exciting pulse and the penetration depth of polaritons in the resonant optical medium.

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

Megala, M.; Rajkumar, Beulah J. M., E-mail: beulah-rajkumar@yahoo.co.in

The electronic and optical transfer properties of Benzene, Benzoic Acid (BA), Nitrobenzene (NB) and Para Nitro Benzoic Acid (PNBA) at ground and first excited state has been investigated by the Density functional theory (DFT)and Time Dependent Density Functional Theory (TDDFT) using SVWN functional/3-21G basis set respectively. Possible intra-molecular charge transfer and n to π* transitions in the ground and the first excitation states have been predicted by the molecular orbitals and the Natural Bond Orbital (NBO) analysis. The simulated absorption spectra have been generated and the result compared with existing experimental results.

Nanometric summation architecture based on optical near-field interaction between quantum dots.

PubMed

Naruse, Makoto; Miyazaki, Tetsuya; Kubota, Fumito; Kawazoe, Tadashi; Kobayashi, Kiyoshi; Sangu, Suguru; Ohtsu, Motoichi

2005-01-15

A nanoscale data summation architecture is proposed and experimentally demonstrated based on the optical near-field interaction between quantum dots. Based on local electromagnetic interactions between a few nanometric elements via optical near fields, we can combine multiple excitations at a certain quantum dot, which allows construction of a summation architecture. Summation plays a key role for content-addressable memory, which is one of the most important functions in optical networks.

Transient photothermal spectra of plasmonic nanobubbles.

PubMed

Lukianova-Hleb, Ekaterina Y; Sassaroli, Elisabetta; Jones, Alicia; Lapotko, Dmitri O

2012-03-13

The photothermal efficacy of near-infrared gold nanoparticles (NP), nanoshells, and nanorods was studied under pulsed high-energy optical excitation in plasmonic nanobubble (PNB) mode as a function of the wavelength and duration of the excitation laser pulse. PNBs, transient vapor nanobubbles, were generated around individual and clustered overheated NPs in water and living cells. Transient PNBs showed two photothermal features not previously observed for NPs: the narrowing of the spectral peaks to 1 nm and the strong dependence of the photothermal efficacy upon the duration of the laser pulse. Narrow red-shifted (relative to those of NPs) near-infrared spectral peaks were observed for 70 ps excitation laser pulses, while longer sub- and nanosecond pulses completely suppressed near-infrared peaks and blue shifted the PNB generation to the visual range. Thus, PNBs can provide superior spectral selectivity over gold NPs under specific optical excitation conditions.

Remote Optical Switch for Localized and Selective Control of Gene Interference

PubMed Central

Lee, Somin Eunice; Liu, Gang Logan; Kim, Franklin; Lee, Luke P.

2009-01-01

Near infrared-absorbing gold nanoplasmonic particles (GNPs) are used as optical switches of gene interference and are remotely controlled using light. We have tuned optical switches to a wavelength where cellular photodamage is minimized. Optical switches are functionalized with double-stranded oligonucleotides. At desired times and at specific intracellular locations, remote optical excitation is used to liberate gene-interfering oligonucleotides. We demonstrate a novel gene-interfering technique offering spatial and temporal control, which is otherwise impossible using conventional gene-interfering techniques. PMID:19128006

Design, assembly, and metrology of an oil-immersion microscope objective with long working distance

NASA Astrophysics Data System (ADS)

Peng, Wei-Jei; Lin, Wen-Lung; Kuo, Hui-Jean; Ho, Cheng-Fang; Hsu, Wei-Yao

2016-10-01

The design, tolerance sensitivity reduction, assembly, and optical bench test for an oil-immersion microscope objective with long working distance employed in a lattice light-sheet microscope is presented in this paper. In this application, the orthogonal excitation and detection objectives are dipped in an oil medium. The excitation objective focuses the incident laser beam to generate fluorescence on specimen for collecting by detection objective. The excitation objective is custom-designed to meet the requirement specification such as oil-immersion, the long working distance, and numerical aperture (NA) of 0.5, etc. To produce an acceptable point spread function (PSF) for effective excitation, the performance of the objective needs to be close to diffraction limit. Because the tolerance of the modulation transfer function (MTF) is more and more sensitive at higher spatial frequency, it is extremely critical to keep the performance after manufacture. Consequently, an insensitive optical design is very important for relaxing tolerance. We compare the design with and without tolerance sensitivity reduction, and the as-built MTF shows the result. Furthermore, the method for sensitivity reduction is presented. The opto-mechanical design and assembly method are also discussed. Eventually, the objective with five spherical lenses was fabricated. In optical bench test, the depth of the oil is sensitive to MTF, and it leads to the complicated adjustment. For solving this issue, we made an index-matching lens to replace oil for measurement easily. Finally, the measured MTF of the excitation objective can accomplish the requirement specification and successfully employed in a lattice light-sheet microscope.

Boric-Acid-Functional Lanthanide Metal-Organic Frameworks for Selective Ratiometric Fluorescence Detection of Fluoride Ions.

PubMed

Yang, Zhong-Rui; Wang, Man-Man; Wang, Xue-Sheng; Yin, Xue-Bo

2017-02-07

Here, we report that boric acid is used to tune the optical properties of lanthanide metal-organic frameworks (LMOFs) for dual-fluorescence emission and improves the selectivity of LMOFs for the determination of F - ions. The LMOFs are prepared with 5-boronoisophthalic acid (5-bop) and Eu 3+ ions as the precursors. Emission mechanism study indicates that 5-bop is excited with UV photons to produce its triplet state, which then excites Eu 3+ ions for their red emission. This is the general story of the antenna effect, but electron-deficient boric acid decreases the energy transfer efficiency from the triplet state of 5-bop to Eu 3+ ions, so dual emission from both 5-bop and Eu 3+ ions is efficiently excited at the single excitation of 275 nm. Moreover, boric acid is used to identify fluoride specifically as a free accessible site. The ratiometric fluorescent detection of F - ions is validated with the dual emission at single excitation. The LMOFs are very monodisperse, so the determination of aqueous F - ions is easily achieved with high selectivity and a low detection limit (2 μM). For the first time, we reveal that rational selection of functional ligands can improve the sensing efficiency of LMOFs through tuning their optical property and enhancing the selectivity toward targets.

Mass transport on adsorbate multilayers studied by surface plasmon polariton wave excitation

NASA Astrophysics Data System (ADS)

Wang, X.; Fei, Y. Y.; Zhu, X. D.

2011-12-01

We excited surface-plasmon polariton waves (SPPW) on Cu(111) by coupling a monochromatic optical beam with a xenon multilayer thickness grating on the metal. The SPPW excitation was detected with an angle-resolved oblique-incidence reflectivity difference technique (OI-RD). The amplitude of the resonance OI-RD signal was a quadratic function of the grating modulation depth. By monitoring the decay of the resonance OI-RD signal as a function of time and temperature, we were able to study the mass transport of xenon that plays a key role in the annealing of a "rough" Xe multilayer crystalline film.

Prediction of Excitation Energies for Conjugated Oligomers and Polymers from Time-Dependent Density Functional Theory

PubMed Central

Tao, Jianmin; Tretiak, Sergei; Zhu, Jian-Xin

2010-01-01

With technological advances, light-emitting conjugated oligomers and polymers have become competitive candidates in the commercial market of light-emitting diodes for display and other technologies, due to the ultralow cost, light weight, and flexibility. Prediction of excitation energies of these systems plays a crucial role in the understanding of their optical properties and device design. In this review article, we discuss the calculation of excitation energies with time-dependent density functional theory, which is one of the most successful methods in the investigation of the dynamical response of molecular systems to external perturbation, owing to its high computational efficiency.

Linked-cluster formulation of electron-hole interaction kernel in real-space representation without using unoccupied states.

PubMed

Bayne, Michael G; Scher, Jeremy A; Ellis, Benjamin H; Chakraborty, Arindam

2018-05-21

Electron-hole or quasiparticle representation plays a central role in describing electronic excitations in many-electron systems. For charge-neutral excitation, the electron-hole interaction kernel is the quantity of interest for calculating important excitation properties such as optical gap, optical spectra, electron-hole recombination and electron-hole binding energies. The electron-hole interaction kernel can be formally derived from the density-density correlation function using both Green's function and TDDFT formalism. The accurate determination of the electron-hole interaction kernel remains a significant challenge for precise calculations of optical properties in the GW+BSE formalism. From the TDDFT perspective, the electron-hole interaction kernel has been viewed as a path to systematic development of frequency-dependent exchange-correlation functionals. Traditional approaches, such as MBPT formalism, use unoccupied states (which are defined with respect to Fermi vacuum) to construct the electron-hole interaction kernel. However, the inclusion of unoccupied states has long been recognized as the leading computational bottleneck that limits the application of this approach for larger finite systems. In this work, an alternative derivation that avoids using unoccupied states to construct the electron-hole interaction kernel is presented. The central idea of this approach is to use explicitly correlated geminal functions for treating electron-electron correlation for both ground and excited state wave functions. Using this ansatz, it is derived using both diagrammatic and algebraic techniques that the electron-hole interaction kernel can be expressed only in terms of linked closed-loop diagrams. It is proved that the cancellation of unlinked diagrams is a consequence of linked-cluster theorem in real-space representation. The electron-hole interaction kernel derived in this work was used to calculate excitation energies in many-electron systems and results were found to be in good agreement with the EOM-CCSD and GW+BSE methods. The numerical results highlight the effectiveness of the developed method for overcoming the computational barrier of accurately determining the electron-hole interaction kernel to applications of large finite systems such as quantum dots and nanorods.

Ultrafast photocarrier dynamics related to defect states of Si1-xGex nanowires measured by optical pump-THz probe spectroscopy.

PubMed

Bae, Jung Min; Lee, Woo-Jung; Jung, Seonghoon; Ma, Jin Won; Jeong, Kwang-Sik; Oh, Seung Hoon; Kim, Seongsin M; Suh, Dongchan; Song, Woobin; Kim, Sunjung; Park, Jaehun; Cho, Mann-Ho

2017-06-14

Slightly tapered Si 1-x Ge x nanowires (NWs) (x = 0.29-0.84) were synthesized via a vapor-liquid-solid procedure using Au as a catalyst. We measured the optically excited carrier dynamics of Si 1-x Ge x NWs as a function of Ge content using optical pump-THz probe spectroscopy. The measured -ΔT/T 0 signals of Si 1-x Ge x NWs were converted into conductivity in the THz region. We developed a fitting formula to apply to indirect semiconductors such as Si 1-x Ge x , which explains the temporal population of photo-excited carriers in the band structure and the relationship between the trapping time and the defect states on an ultrafast time scale. From the fitting results, we extracted intra- and inter-valley transition times and trapping times of electrons and holes of Si 1-x Ge x NWs as a function of Ge content. On the basis of theoretical reports, we suggest a physical model to interpret the trapping times related to the species of interface defect states located at the oxide/NW: substoichiometric oxide states of Si(Ge) 0+,1+,2+ , but not Si(Ge) 3+ , could function as defect states capturing photo-excited electrons or holes and could determine the different trapping times of electrons and holes depending on negatively or neutrally charged states.

Plane-Wave Implementation and Performance of à-la-Carte Coulomb-Attenuated Exchange-Correlation Functionals for Predicting Optical Excitation Energies in Some Notorious Cases.

PubMed

Bircher, Martin P; Rothlisberger, Ursula

2018-06-12

Linear-response time-dependent density functional theory (LR-TD-DFT) has become a valuable tool in the calculation of excited states of molecules of various sizes. However, standard generalized-gradient approximation and hybrid exchange-correlation (xc) functionals often fail to correctly predict charge-transfer (CT) excitations with low orbital overlap, thus limiting the scope of the method. The Coulomb-attenuation method (CAM) in the form of the CAM-B3LYP functional has been shown to reliably remedy this problem in many CT systems, making accurate predictions possible. However, in spite of a rather consistent performance across different orbital overlap regimes, some pitfalls remain. Here, we present a fully flexible and adaptable implementation of the CAM for Γ-point calculations within the plane-wave pseudopotential molecular dynamics package CPMD and explore how customized xc functionals can improve the optical spectra of some notorious cases. We find that results obtained using plane waves agree well with those from all-electron calculations employing atom-centered bases, and that it is possible to construct a new Coulomb-attenuated xc functional based on simple considerations. We show that such a functional is able to outperform CAM-B3LYP in some cases, while retaining similar accuracy in systems where CAM-B3LYP performs well.

Excitation mechanisms of Er optical centers in GaN epilayers

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

George, D. K.; Hawkins, M. D.; McLaren, M.

2015-10-26

We report direct evidence of two mechanisms responsible for the excitation of optically active Er{sup 3+} ions in GaN epilayers grown by metal-organic chemical vapor deposition. These mechanisms, resonant excitation via the higher-lying inner 4f shell transitions and band-to-band excitation of the semiconductor host, lead to narrow emission lines from isolated and the defect-related Er optical centers. However, these centers have different photoluminescence spectra, local defect environments, decay dynamics, and excitation cross sections. The photoluminescence at 1.54 μm from the isolated Er optical center which can be excited by either mechanism has the same decay dynamics, but possesses a much highermore » excitation cross-section under band-to-band excitation. In contrast, the photoluminescence at 1.54 μm from the defect-related Er optical center can only be observed through band-to-band excitation but has the largest excitation cross-section. These results explain the difficulty in achieving gain in Er doped GaN and indicate approaches for realization of optical amplification, and possibly lasing, at room temperature.« less

Optical properties, excitation energy and primary charge transfer in photosystem II: theory meets experiment.

PubMed

Renger, Thomas; Schlodder, Eberhard

2011-01-01

In this review we discuss structure-function relationships of the core complex of photosystem II, as uncovered from analysis of optical spectra of the complex and its subunits. Based on descriptions of optical difference spectra including site directed mutagenesis we propose a revision of the multimer model of the symmetrically arranged reaction center pigments, described by an asymmetric exciton Hamiltonian. Evidence is provided for the location of the triplet state, the identity of the primary electron donor, the localization of the cation and the secondary electron transfer pathway in the reaction center. We also discuss the stationary and time-dependent optical properties of the CP43 and CP47 subunits and the excitation energy transfer and trapping-by-charge-transfer kinetics in the core complex. Copyright © 2011 Elsevier B.V. All rights reserved.

Transverse optic-like modes in binary liquids

NASA Astrophysics Data System (ADS)

Bryk, Taras; Mryglod, Ihor

1999-10-01

Generalized collective mode approach and MD simulations are applied for the study of transverse dynamics in a LJ fluid KrAr and a liquid alloy Mg 70Zn 30. The optic-like excitations, caused by the mass-concentration fluctuations, are found in both mixtures considered. Mode contributions into the total spectral function are investigated.

Improving the precision of linear optics measurements based on turn-by-turn beam position monitor data after a pulsed excitation in lepton storage rings

NASA Astrophysics Data System (ADS)

Malina, L.; Coello de Portugal, J.; Persson, T.; Skowroński, P. K.; Tomás, R.; Franchi, A.; Liuzzo, S.

2017-08-01

Beam optics control is of critical importance for machine performance and protection. Nowadays, turn-by-turn (TbT) beam position monitor (BPM) data are increasingly exploited as they allow for fast and simultaneous measurement of various optics quantities. Nevertheless, so far the best documented uncertainty of measured β -functions is of about 10‰ rms. In this paper we compare the β -functions of the ESRF storage ring measured from two different TbT techniques—the N-BPM and the Amplitude methods—with the ones inferred from a measurement of the orbit response matrix (ORM). We show how to improve the precision of TbT techniques by refining the Fourier transform of TbT data with properly chosen excitation amplitude. The precision of the N-BPM method is further improved by refining the phase advance measurement. This represents a step forward compared to standard TbT measurements. First experimental results showing the precision of β -functions pushed down to 4‰ both in TbT and ORM techniques are reported and commented.

Hotspot relaxation dynamics in a current-carrying superconductor

NASA Astrophysics Data System (ADS)

Marsili, F.; Stevens, M. J.; Kozorezov, A.; Verma, V. B.; Lambert, Colin; Stern, J. A.; Horansky, R. D.; Dyer, S.; Duff, S.; Pappas, D. P.; Lita, A. E.; Shaw, M. D.; Mirin, R. P.; Nam, S. W.

2016-03-01

We experimentally studied the dynamics of optically excited hotspots in current-carrying WSi superconducting nanowires as a function of bias current, bath temperature, and excitation wavelength. We observed that the hotspot relaxation time depends on bias current, temperature, and wavelength. We explained this effect with a model based on quasiparticle recombination, which provides insight into the quasiparticle dynamics of superconductors.

Optical polarization based logic functions (XOR or XNOR) with nonlinear Gallium nitride nanoslab.

PubMed

Bovino, F A; Larciprete, M C; Giardina, M; Belardini, A; Centini, M; Sibilia, C; Bertolotti, M; Passaseo, A; Tasco, V

2009-10-26

We present a scheme of XOR/XNOR logic gate, based on non phase-matched noncollinear second harmonic generation from a medium of suitable crystalline symmetry, Gallium nitride. The polarization of the noncollinear generated beam is a function of the polarization of both pump beams, thus we experimentally investigated all possible polarization combinations, evidencing that only some of them are allowed and that the nonlinear interaction of optical signals behaves as a polarization based XOR. The experimental results show the peculiarity of the nonlinear optical response associated with noncollinear excitation, and are explained using the expression for the effective second order optical nonlinearity in noncollinear scheme.

Fluorescence lifetime measurements in heterogeneous scattering medium

NASA Astrophysics Data System (ADS)

Nishimura, Goro; Awasthi, Kamlesh; Furukawa, Daisuke

2016-07-01

Fluorescence lifetime in heterogeneous multiple light scattering systems is analyzed by an algorithm without solving the diffusion or radiative transfer equations. The algorithm assumes that the optical properties of medium are constant in the excitation and emission wavelength regions. If the assumption is correct and the fluorophore is a single species, the fluorescence lifetime can be determined by a set of measurements of temporal point-spread function of the excitation light and fluorescence at two different concentrations of the fluorophore. This method is not dependent on the heterogeneity of the optical properties of the medium as well as the geometry of the excitation-detection on an arbitrary shape of the sample. The algorithm was validated by an indocyanine green fluorescence in phantom measurements and demonstrated by an in vivo measurement.

New insight into the spin-conserving excitation of the negatively charged nitrogen-vacancy center in diamond

PubMed Central

Deng, Bei; Zhang, R. Q.; Shi, X. Q.

2014-01-01

The negatively charged nitrogen-vacancy (N-V−) color center in diamond is an important solid-state single photon source for applications to quantum communication and distributed quantum computation. Its full usefulness relies on sufficient radiative emission of the optical photons which requires realizable control to enhance emission into the zero-phonon line (ZPL) but until now is still a challenge. Detailed understanding of the associated excitation process would be of essential importance for such objective. Here we report a theoretical work that probes the spin-conserving optical excitation of the N-V− center. Using density-functional-theory (DFT) calculations, we find that the ZPL and the phonon-side band (PSB) depend sensitively on the axial strain of the system. Besides, we find a relatively small PSB appearing at about 100 GPa in the emission spectrum at low temperatures, which provides a means to enhance the coherent emission of the N-V− center in quantum optical networks. PMID:24888367

Endoscopic tissue autofluorescence measurements in the upper aerodigestive tract and the bronchi

NASA Astrophysics Data System (ADS)

Braichotte, Daniel; Wagnieres, Georges A.; Monnier, Philippe; Savary, Jean-Francois; Bays, Roland; van den Bergh, Hubert; Chatelain, Andre

1991-11-01

A single multimode optical fiber is used to excite and collect tissue autofluorescence as well as the fluorescence of an IV-injected fluorescent tumor marker. Measurements of the relative fluorescence intensity of a tumor marker as a function of the time after IV injection permit measurement of the kinetics of this substance in tumor, normal tissue, and skin. The authors believe that these are the first measurements of this kind in patients. Furthermore, the autofluorescence spectrum generated at several excitation wavelengths in different tissues is compared, for instance in the oesophagus, the bronchi, and the tongue. The measuring system is based on an optical multichannel analyzer which measures the fluorescence excited by monochromatic radiation from a spectrally filtered Xe lamp. A correlation between the observed pharmacokinetics and tumor properties like the degree of vascularization is of fundamental importance for each selected tumor marker. Also, the results of these measurements are used for the optical detection of tumors.

Inhomogeneous nuclear spin polarization induced by helicity-modulated optical excitation of fluorine-bound electron spins in ZnSe

NASA Astrophysics Data System (ADS)

Heisterkamp, F.; Greilich, A.; Zhukov, E. A.; Kirstein, E.; Kazimierczuk, T.; Korenev, V. L.; Yugova, I. A.; Yakovlev, D. R.; Pawlis, A.; Bayer, M.

2015-12-01

Optically induced nuclear spin polarization in a fluorine-doped ZnSe epilayer is studied by time-resolved Kerr rotation using resonant excitation of donor-bound excitons. Excitation with helicity-modulated laser pulses results in a transverse nuclear spin polarization, which is detected as a change of the Larmor precession frequency of the donor-bound electron spins. The frequency shift in dependence on the transverse magnetic field exhibits a pronounced dispersion-like shape with resonances at the fields of nuclear magnetic resonance of the constituent zinc and selenium isotopes. It is studied as a function of external parameters, particularly of constant and radio frequency external magnetic fields. The width of the resonance and its shape indicate a strong spatial inhomogeneity of the nuclear spin polarization in the vicinity of a fluorine donor. A mechanism of optically induced nuclear spin polarization is suggested based on the concept of resonant nuclear spin cooling driven by the inhomogeneous Knight field of the donor-bound electron.

Fluorescent fluid interface position sensor

DOEpatents

Weiss, Jonathan D.

2004-02-17

A new fluid interface position sensor has been developed, which is capable of optically determining the location of an interface between an upper fluid and a lower fluid, the upper fluid having a larger refractive index than a lower fluid. The sensor functions by measurement, of fluorescence excited by an optical pump beam which is confined within a fluorescent waveguide where that waveguide is in optical contact with the lower fluid, but escapes from the fluorescent waveguide where that waveguide is in optical contact with the upper fluid.

Spatially confined low-power optically pumped ultrafast synchrotron x-ray nanodiffraction

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

Park, Joonkyu; Zhang, Qingteng; Chen, Pice

2015-08-27

The combination of ultrafast optical excitation and time-resolved synchrotron x-ray nanodiffraction provides unique insight into the photoinduced dynamics of materials, with the spatial resolution required to probe individual nanostructures or small volumes within heterogeneous materials. Optically excited x-ray nanobeam experiments are challenging because the high total optical power required for experimentally relevant optical fluences leads to mechanical instability due to heating. For a given fluence, tightly focusing the optical excitation reduces the average optical power by more than three orders of magnitude and thus ensures sufficient thermal stability for x-ray nanobeam studies. Delivering optical pulses via a scannable fiber-coupled opticalmore » objective provides a well-defined excitation geometry during rotation and translation of the sample and allows the selective excitation of isolated areas within the sample. Finally, experimental studies of the photoinduced lattice dynamics of a 35 nm BiFeO 3 thin film on a SrTiO 3 substrate demonstrate the potential to excite and probe nanoscale volumes.« less

Micromanipulation and physiological monitoring of cells using two-photon excited fluorescence in cw laser tweezers

NASA Astrophysics Data System (ADS)

Sonek, Gregory J.; Liu, Yagang; Berns, Michael W.; Tromberg, Bruce J.

1996-05-01

We report the observation of two-photon fluorescence excitation and cell confinement, simultaneously, in a continuous-wave (cw) single-beam gradient force optical trap, and demonstrate its use as an in-situ probe to study the physiological state of an optically confined cell sample. At the wavelength of 1064 nm, a single focused gaussian laser beam is used to simultaneously confine, and excite visible fluorescence from, a human sperm cell that has been tagged with propidium iodide, a exogenous fluorescent dye that functions as a viability assay of cellular physiological state. The intensity at the dye peak emission wavelength of 620 nm exhibits a near-square-law dependence on incident trapping beam photon laser power, a behavior consistent with a two-photon absorption process. In addition, for a sperm cell held stationary in the optical tweezers for a period of several minutes at a constant trapping power, red fluorescence emission was observed to increase the time, indicating that the cell has gradually transitioned between a live and dead state. Two-photon excited fluorescence was also observed in chinese hamster ovary cells that were confined by cw laser tweezers and stained with either propidium iodide or Snarf, a pH-sensitive dye probe. These results suggest that, for samples suitably tagged with fluorescent probes and vital stains, optical tweezers can be used to generate their own in-situ diagnostic optical probes of cellular viability or induced photodamage, via two-photon processes.

Multiple excitation nano-spot generation and confocal detection for far-field microscopy.

PubMed

Mondal, Partha Pratim

2010-03-01

An imaging technique is developed for the controlled generation of multiple excitation nano-spots for far-field microscopy. The system point spread function (PSF) is obtained by interfering two counter-propagating extended depth-of-focus PSF (DoF-PSF), resulting in highly localized multiple excitation spots along the optical axis. The technique permits (1) simultaneous excitation of multiple planes in the specimen; (2) control of the number of spots by confocal detection; and (3) overcoming the point-by-point based excitation. Fluorescence detection from the excitation spots can be efficiently achieved by Z-scanning the detector/pinhole assembly. The technique complements most of the bioimaging techniques and may find potential application in high resolution fluorescence microscopy and nanoscale imaging.

Multiple excitation nano-spot generation and confocal detection for far-field microscopy

NASA Astrophysics Data System (ADS)

Mondal, Partha Pratim

2010-03-01

An imaging technique is developed for the controlled generation of multiple excitation nano-spots for far-field microscopy. The system point spread function (PSF) is obtained by interfering two counter-propagating extended depth-of-focus PSF (DoF-PSF), resulting in highly localized multiple excitation spots along the optical axis. The technique permits (1) simultaneous excitation of multiple planes in the specimen; (2) control of the number of spots by confocal detection; and (3) overcoming the point-by-point based excitation. Fluorescence detection from the excitation spots can be efficiently achieved by Z-scanning the detector/pinhole assembly. The technique complements most of the bioimaging techniques and may find potential application in high resolution fluorescence microscopy and nanoscale imaging.

Force-detected nanoscale absorption spectroscopy in water at room temperature using an optical trap

NASA Astrophysics Data System (ADS)

Parobek, Alexander; Black, Jacob W.; Kamenetska, Maria; Ganim, Ziad

2018-04-01

Measuring absorption spectra of single molecules presents a fundamental challenge for standard transmission-based instruments because of the inherently low signal relative to the large background of the excitation source. Here we demonstrate a new approach for performing absorption spectroscopy in solution using a force measurement to read out optical excitation at the nanoscale. The photoinduced force between model chromophores and an optically trapped gold nanoshell has been measured in water at room temperature. This photoinduced force is characterized as a function of wavelength to yield the force spectrum, which is shown to be correlated to the absorption spectrum for four model systems. The instrument constructed for these measurements combines an optical tweezer with frequency domain absorption spectroscopy over the 400-800 nm range. These measurements provide proof-of-principle experiments for force-detected nanoscale spectroscopies that operate under ambient chemical conditions.

Excited-state absorption in tetrapyridyl porphyrins: comparing real-time and quadratic-response time-dependent density functional theory

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

Bowman, David N.; Asher, Jason C.; Fischer, Sean A.

2017-01-01

Threemeso-substituted tetrapyridyl porphyrins (free base, Ni(ii), and Cu(ii)) were investigated for their optical limiting (OL) capabilities using real-time (RT-), linear-response (LR-), and quadratic-response (QR-) time-dependent density functional theory (TDDFT) methods.

Self-pulsations and excitability in optically injected quantum-dot lasers: Impact of the excited states and spontaneous emission noise

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

Olejniczak, Lukasz; SUPELEC, OPTEL, and LMOPS EA 4423; Panajotov, Krassimir

2010-08-15

We study the dynamics of an optically injected quantum-dot laser accounting for excited states. Mapping of the bifurcations in the plane frequency detuning vs. injection strength shows that the relaxation rate scales the regions of locking and single- and double-period solutions, while the capture rate has a minor effect. Within the regions of time-periodic solutions, close to the saddle-node bifurcation boundary, we identify subregions where the output signal resembles excitable pulses as a result of the bottleneck phenomenon. We show that such emission is determined mainly by fluctuations in the occupation of the excited states. The interpulse time follows anmore » inverse square root scaling law as a function of the detuning. In a deterministic system the pulses are periodic regardless of the detuning, but in the presence of noise, close to the locking region, the interpulse time follows a positively skewed normal distribution. For a fixed frequency detuning, increasing the noise strength can shift the mean of the interpulse time distribution and make the pulsations more periodic.« less

Physical Meaning of Virtual Kohn-Sham Orbitals and Orbital Energies: An Ideal Basis for the Description of Molecular Excitations.

PubMed

van Meer, R; Gritsenko, O V; Baerends, E J

2014-10-14

In recent years, several benchmark studies on the performance of large sets of functionals in time-dependent density functional theory (TDDFT) calculations of excitation energies have been performed. The tested functionals do not approximate exact Kohn-Sham orbitals and orbital energies closely. We highlight the advantages of (close to) exact Kohn-Sham orbitals and orbital energies for a simple description, very often as just a single orbital-to-orbital transition, of molecular excitations. Benchmark calculations are performed for the statistical average of orbital potentials (SAOP) functional for the potential [J. Chem. Phys. 2000, 112, 1344; 2001, 114, 652], which approximates the true Kohn-Sham potential much better than LDA, GGA, mGGA, and hybrid potentials do. An accurate Kohn-Sham potential does not only perform satisfactorily for calculated vertical excitation energies of both valence and Rydberg transitions but also exhibits appealing properties of the KS orbitals including occupied orbital energies close to ionization energies, virtual-occupied orbital energy gaps very close to excitation energies, realistic shapes of virtual orbitals, leading to straightforward interpretation of most excitations as single orbital transitions. We stress that such advantages are completely lost in time-dependent Hartree-Fock and partly in hybrid approaches. Many excitations and excitation energies calculated with local density, generalized gradient, and hybrid functionals are spurious. There is, with an accurate KS, or even the LDA or GGA potentials, nothing problematic about the "band gap" in molecules: the HOMO-LUMO gap is close to the first excitation energy (the optical gap).

Crystallochromy of perylene pigments: Interference between Frenkel excitons and charge-transfer states

NASA Astrophysics Data System (ADS)

Gisslén, Linus; Scholz, Reinhard

2009-09-01

The optical properties of perylene-based pigments are arising from the interplay between neutral molecular excitations and charge transfer between adjacent molecules. In the crystalline phase, these excitations are coupled via electron and hole transfer, two quantities relating directly to the width of the conduction and valence band in the crystalline phase. Based on the crystal structure determined by x-ray diffraction, density-functional theory (DFT) and Hartree-Fock are used for the calculation of the electronic states of a dimer of stacked molecules. The resulting transfer parameters for electron and hole are used in an exciton model for the coupling between Frenkel excitons and charge-transfer states. The deformation of the positively or negatively charged molecular ions with respect to the neutral ground state is calculated with DFT and the geometry in the optically excited state is deduced from time-dependent DFT and constrained DFT. All of these deformations are interpreted in terms of the elongation of an effective internal vibration which is used subsequently in the exciton model for the crystalline phase. A comparison between the calculated dielectric function and the observed optical spectra allows to deduce the relative energetic position of Frenkel excitons and the charge-transfer state involving stack neighbors, a key parameter for various electronic and optoelectronic device applications. For five out of six perylene pigments studied in the present work, this exciton model results in excellent agreement between calculated and observed optical properties.

Dynamics of Nonlinear Excitation of the High-Order Mode in a Single-Mode Step-Index Optical Fiber

NASA Astrophysics Data System (ADS)

Burdin, V.; Bourdine, A.

2018-04-01

This work is concerned with approximate model of higher-order mode nonlinear excitation in a singlemode silica optical fiber. We present some results of simulation for step-index optical fiber under femtosecond optical pulse launching, which confirm ability of relatively stable higher-order mode excitation in such singlemode optical fiber over sufficiently narrow range of launched optical power variation.

Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons

PubMed Central

Soavi, Giancarlo; Dal Conte, Stefano; Manzoni, Cristian; Viola, Daniele; Narita, Akimitsu; Hu, Yunbin; Feng, Xinliang; Hohenester, Ulrich; Molinari, Elisa; Prezzi, Deborah; Müllen, Klaus; Cerullo, Giulio

2016-01-01

Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron–hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton–exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ≈250 meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. These observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics. PMID:26984281

The pseudogap and the unusual excitations in the optical conductivity of Bi2Sr2CaCu2O8+δ material

NASA Astrophysics Data System (ADS)

Bhuiyan, E. H.; Azzouz, M.

2017-12-01

We studied the optical conductivity of Bi2Sr2CaCu2O8+δ material as a function of temperature and doping within the Rotating Antiferromagnetism Theory (RAFT). The optical conductivity of the material is studied from underdoped to overdoped regime for a wide range of temperatures. We mainly focused on the pseudogap state and unusual excitations in the optical conductivity. The former is realized in the underdoped to optimally doped regimes below a characteristic temperature T*, a temperature that can appreciably exceed the superconducting transition temperature TC. The latter is appeared in the optical conductivity spectra below the TC and we studied it by varying temperature. The pseudogap response is explored by changing the doping level and by varying the temperature from above to below T*. The results obtained from theories are compared with available experimental data and found a good agreement with those experimental results.

Fiber optic immunosensor for cross-linked fibrin concentration

NASA Astrophysics Data System (ADS)

Moskowitz, Samuel E.

2000-08-01

Working with calcium ions in the blood, platelets produce thromboplastin which transforms prothrombin into thrombin. Removing peptides, thrombin changes fibrinogen into fibrin. Cross-linked insoluble fibrin polymers are solubilized by enzyme plasmin found in blood plasma. Resulting D-dimers are elevated in patients with intravascular coagulation, deep venous thrombosis, pulmonary embolism, myocardial infarction, multiple trauma, cancer, impaired renal and liver functions, and sepsis. Consisting principally of a NIR 780 nm GaAlAs laser diode and a 800 nm avalanche photodiode (APD), the fiber-optic immunosensor can determined D-dimer concentration to levels <0.1 ng/ml. A capture monoclonal antibody to the antigen soluble cross-linked fibrin is employed. Immobilized at the tip of an optical fiber by avidin-biotin, the captured antigen is detected by a second antibody which is labeled with NN 382 fluorescent dye. An evanescent wave traveling on an excitation optical fiber excites the antibody-antigen fluorophore complex. Concentration of cross-linked fibrin is directly proportional to the APD measured intensity of fluorescence. NIR fluorescence has advantages of low background interference, short fluorescence lifetime, and large difference between excitation and emission peaks. Competitive ELISA test for D-dimer concentration requires trained personnel performing a time consuming operation.

Nonlinear optical effects in semi-polar GaN micro-cavity emitter

NASA Astrophysics Data System (ADS)

Butler, Sween; Jiang, Hongxing; Lin, Jingyu; Neogi, Arup

Nonlinear optical (NLO) response of low dimensional emitters is of current interest because of the need for active elements in photonic applications. NLO effects in a selectively grown array of semi-polar GaN microcavity structures offer a promising route toward devices for integrated optical circuitry in optoelectronics and photonics field. Localized spatial excitation of a single hexagonal GaN microcavity with semipolar facets formed by selective area growth was optimized for nonlinear optical light generation due to second harmonic generation (SHG) and multi-photon luminescence(MPL). Multi-photon transition induced by tightly focused femtosecond NIR incident field results in ultra-violet and yellow luminescence for excitations above and below half bandgap energy, whereas SHG was observed for below half bandgap energy. We show that color and coherence of the light generation from the emitter can be controlled by selective onset of the nonlinear process which depends not only on the incident laser energy and intensity but also on the geometry of the microcavity. Quasi-WGM like modes were observed for off-resonant excitations from the GaN microcavity resulting in enhanced SHG. The directionality of MPL and SHG will be presented as a function of the pump polarization.

Nonlinear Optical Properties of Bacteriorhodopsin and Retinal Chromophores and Their Applications for Optical Information Storage and Processing.

NASA Astrophysics Data System (ADS)

Chen, Zhongping

Retinal, a conjugated polyene, plays a crucial role in biology. Both the visual pigments and the energy transducing protein, bacteriorhodopsin (BR) have a form of retinal as their chromophores. Because visual excitation and energy transduction in these systems is initiated by the promotion of retinal to an excited electronic state, information about the excited-state structure of retinal and the effect of chromophore/protein interactions on this structure are essential to understanding the functions of these systems. In this thesis, surface second harmonic (SH) generation is used to measure the light-induced dipole moment changes of a series of retinal derivatives that were designed and synthesized to model specific components of chromophore/protein interactions. In addition, we report an in situ probe of the dipole moment change of the retinal chromophore bound in BR by SH generation from oriented purple membranes. The dipole moment changes of various forms of BR, including light-adapted, dark-adapted, blue, and acid purple membrane, were measured and compared. These results, combined with the results from model compounds, elucidate the effects of the chromophore/protein interactions on light-induced charge redistribution and give insight on the fundamental nature of light excitation and energy storage in SR and rhodopsin. Furthermore, the dependence of the molecular hyperpolarizability of the conjugated molecules on donor/acceptor strength, protonation, conjugate length, planarity, and nonconjugate charges is investigated. Our study shows for the first time that nonconjugated charges have a very large effect on the nonlinear optical properties of conjugated molecules. BR has interesting photochromic characteristics, very large optical nonlinearities, and a unique optoelectrical property where the polarity of the photovoltage depends on both its photochromic state and the excitation wavelength. These unique characteristics coupled with its high stability make BR an important biological material for optical information processing and storage. Erasable optical storage with three-dimensional capacity and optical implementation of neural networks using SR are reported in this thesis. Oriented BR-polymer films with excellent optical qualities and stable photochromic states are developed, and nondestructive reading of stored information using SH generation is proposed and demonstrated.

Dissociative excitation of the manganese atom quartet levels by collisions e-MnBr2

NASA Astrophysics Data System (ADS)

Smirnov, Yu M.

2017-04-01

Dissociative excitation of quartet levels of the manganese atom was studied in collisions of electrons with manganese dibromide molecules. Eighty-two cross-sections for transitions originating at odd levels and eleven cross-sections for transitions originating at even levels have been measured at an incident electron energy of 100 eV. An optical excitation function has been recorded in the electron energy range of 0-100 eV for transitions originating from 3d 64p z 4 F° levels. For the majority of transitions, a comparison of the resulting cross-section values to cross-sections produced by direct excitation is provided.

Theory of spin-conserving excitation of the N-V(-) center in diamond.

PubMed

Gali, Adam; Janzén, Erik; Deák, Péter; Kresse, Georg; Kaxiras, Efthimios

2009-10-30

The negatively charged nitrogen-vacancy defect in diamond is an important atomic-scale structure that can be used as a qubit in quantum computing and as a marker in biomedical applications. Its usefulness relies on the ability to optically excite electrons between well-defined gap states, which requires a clear and detailed understanding of the relevant states and excitation processes. Here we show that by using hybrid density-functional-theory calculations in a large supercell we can reproduce the zero-phonon line and the Stokes and anti-Stokes shifts, yielding a complete picture of the spin-conserving excitation of this defect.

Electronic structure and optical spectra of semiconducting carbon nanotubes functionalized by diazonium salts

NASA Astrophysics Data System (ADS)

Ramirez, Jessica; Mayo, Michael L.; Kilina, Svetlana; Tretiak, Sergei

2013-02-01

We report density functional (DFT) calculations on finite-length semiconducting carbon nanotubes covalently and non-covalently functionalized by aryl diazonium moieties and their chlorinated derivatives. For these systems, we investigate (i) an accuracy of different functionals and basis sets, (ii) a solvent effect, and (iii) the impact of the chemical functionalization on optical properties of nanotubes. In contrast to B3LYP, only long-range-corrected functionals, such as CAM-B3LYP and wB97XD, properly describe the ground and excited state properties of physisorbed molecules. We found that physisorbed cation insignificantly perturbs the optical spectra of nanotubes. In contrast, covalently bound complexes demonstrate strong redshifts and brightening of the lowest exciton that is optically dark in pristine nanotubes. However, the energy and oscillator strength of the lowest state are dictated by the position of the molecule on the nanotube. Thus, if controllable and selective chemical functionalization is realized, the PL of nanotubes could be improved.

Microwave-optical two-photon excitation of Rydberg states

NASA Astrophysics Data System (ADS)

Tate, D. A.; Gallagher, T. F.

2018-03-01

We report efficient microwave-optical two photon excitation of Rb Rydberg atoms in a magneto-optical trap. This approach allows the excitation of normally inaccessible states and provides a path toward excitation of high-angular-momentum states. The efficiency stems from the elimination of the Doppler width, the use of a narrow-band pulsed laser, and the enormous electric-dipole matrix element connecting the intermediate and final states of the transition. The excitation is efficient in spite of the low optical and microwave powers, of order 1 kW and 1 mW, respectively. This is an application of the large dipole coupling strengths between Rydberg states to achieve two-photon excitation of Rydberg atoms.

Optical Imaging and Control of Neurons

NASA Astrophysics Data System (ADS)

Song, Yoon-Kyu

Although remarkable progress has been made in our understanding of the function, organization, and development of the brain by various approaches of modern science and technology, how the brain performs its marvelous function remains unsolved or incompletely understood. This is mainly attributed to the insufficient capability of currently available research tools and conceptual frameworks to deal with enormous complexity of the brain. Hence, in the last couple of decades, a significant effort has been made to crack the complexity of brain by utilizing research tools from diverse scientific areas. The research tools include the optical neurotechnology which incorporates the exquisite characteristics of optics, such as multi-parallel access and non-invasiveness, in sensing and stimulating the excitable membrane of a neuron, the basic functional unit of the brain. This chapter is aimed to serve as a short introduction to the optical neurotechnology for those who wish to use optical techniques as one of their brain research tools.

TD-CI simulation of the electronic optical response of molecules in intense fields II: comparison of DFT functionals and EOM-CCSD.

PubMed

Sonk, Jason A; Schlegel, H Bernhard

2011-10-27

Time-dependent configuration interaction (TD-CI) simulations can be used to simulate molecules in intense laser fields. TD-CI calculations use the excitation energies and transition dipoles calculated in the absence of a field. The EOM-CCSD method provides a good estimate of the field-free excited states but is rather expensive. Linear-response time-dependent density functional theory (TD-DFT) is an inexpensive alternative for computing the field-free excitation energies and transition dipoles needed for TD-CI simulations. Linear-response TD-DFT calculations were carried out with standard functionals (B3LYP, BH&HLYP, HSE2PBE (HSE03), BLYP, PBE, PW91, and TPSS) and long-range corrected functionals (LC-ωPBE, ωB97XD, CAM-B3LYP, LC-BLYP, LC-PBE, LC-PW91, and LC-TPSS). These calculations used the 6-31G(d,p) basis set augmented with three sets of diffuse sp functions on each heavy atom. Butadiene was employed as a test case, and 500 excited states were calculated with each functional. Standard functionals yield average excitation energies that are significantly lower than the EOM-CC, while long-range corrected functionals tend to produce average excitation energies slightly higher. Long-range corrected functionals also yield transition dipoles that are somewhat larger than EOM-CC on average. The TD-CI simulations were carried out with a three-cycle Gaussian pulse (ω = 0.06 au, 760 nm) with intensities up to 1.26 × 10(14) W cm(-2) directed along the vector connecting the end carbons. The nonlinear response as indicated by the residual populations of the excited states after the pulse is far too large with standard functionals, primarily because the excitation energies are too low. The LC-ωPBE, LC-PBE, LC-PW91, and LC-TPSS long-range corrected functionals produce responses comparable to EOM-CC.

Laser pulse induced multi-exciton dynamics in molecular systems

NASA Astrophysics Data System (ADS)

Wang, Luxia; May, Volkhard

2018-03-01

Ultrafast optical excitation of an arrangement of identical molecules is analyzed theoretically. The computations are particularly dedicated to molecules where the excitation energy into the second excited singlet state E(S 2) - E(S 0) is larger than twice the excitation energy into the first excited singlet state E(S 1) - E(S 0). Then, exciton-exciton annihilation is diminished and resonant and intensive excitation may simultaneously move different molecules into their first excited singlet state | {S}1> . To describe the temporal evolution of the thus created multi-exciton state a direct computation of the related wave function is circumvented. Instead, we derive equations of motion for expectation values formed by different arrangements of single-molecule transition operators | {S}1> < {S}0| . First simulation results are presented and the approximate treatment suggested recently in 2016 Phys. Rev. B 94 195413 is evaluated.

Raman Laser Spectrometer internal Optical Head current status: opto-mechanical redesign to minimize the excitation laser trace

NASA Astrophysics Data System (ADS)

Sanz, Miguel; Ramos, Gonzalo; Moral, Andoni; Pérez, Carlos; Belenguer, Tomás; del Rosario Canchal, María; Zuluaga, Pablo; Rodriguez, Jose Antonio; Santiago, Amaia; Rull, Fernando; Instituto Nacional de Técnica Aeroespacial (INTA); Ingeniería de Sistemas para la Defesa de España S.A. (ISDEFE)

2016-10-01

Raman Laser Spectrometer (RLS) is the Pasteur Payload instruments of the ExoMars mission, within the ESA's Aurora Exploration Programme, that will perform for the first time in an out planetary mission Raman spectroscopy. RLS is composed by SPU (Spectrometer Unit), iOH (Internal Optical Head), and ICEU (Instrument Control and Excitation Unit). iOH focuses the excitation laser on the samples (excitation path), and collects the Raman emission from the sample (collection path, composed on collimation system and filtering system). The original design presented a high laser trace reaching to the detector, and although a certain level of laser trace was required for calibration purposes, the high level degrades the Signal to Noise Ratio confounding some Raman peaks.The investigation revealing that the laser trace was not properly filtered as well as the iOH opto-mechanical redesign are reported on. After the study of the Long Pass Filters Optical Density (OD) as a function of the filtering stage to the detector distance, a new set of filters (Notch filters) was decided to be evaluated. Finally, and in order to minimize the laser trace, a new collection path design (mainly consisting on that the collimation and filtering stages are now separated in two barrels, and on the kind of filters to be used) was required. Distance between filters and collimation stage first lens was increased, increasing the OD. With this new design and using two Notch filters, the laser trace was reduced to assumable values, as can be observed in the functional test comparison also reported on this paper.

Delocalized versus localized excitations in the photoisomerization of azobenzene-functionalized alkanethiolate SAMs

NASA Astrophysics Data System (ADS)

Bronsch, Wibke; Moldt, Thomas; Boie, Larissa; Gahl, Cornelius; Weinelt, Martin

2017-12-01

Self-assembled monolayers of azobenzene-functionalized alkanethiolates form molecular ensembles with preferential orientation and significant excitonic coupling among the azobenzene chromophores. We have studied their optical switching with differential reflectance and two-photon-photoemission spectroscopy tuning the excitation wavelength through the excitonically broadened S2 absorption band. While the effective isomerization cross-section increases towards shorter wavelengths, the fraction of cis molecules in the photostationary state decreases. We attribute this observation to the absorption of the cis isomer in the SAM. The photoisomerization in the SAM thereby follows the behavior of non-interacting chromophores in solution, despite the formation of H-aggregates. Our study thus reveals that photoswitching occurs via localized excitations while strongly excitonically coupled, delocalized states do not contribute significantly.

Probing the interatomic potential of solids with strong-field nonlinear phononics

NASA Astrophysics Data System (ADS)

von Hoegen, A.; Mankowsky, R.; Fechner, M.; Först, M.; Cavalleri, A.

2018-03-01

Nonlinear optical techniques at visible frequencies have long been applied to condensed matter spectroscopy. However, because many important excitations of solids are found at low energies, much can be gained from the extension of nonlinear optics to mid-infrared and terahertz frequencies. For example, the nonlinear excitation of lattice vibrations has enabled the dynamic control of material functions. So far it has only been possible to exploit second-order phonon nonlinearities at terahertz field strengths near one million volts per centimetre. Here we achieve an order-of-magnitude increase in field strength and explore higher-order phonon nonlinearities. We excite up to five harmonics of the A1 (transverse optical) phonon mode in the ferroelectric material lithium niobate. By using ultrashort mid-infrared laser pulses to drive the atoms far from their equilibrium positions, and measuring the large-amplitude atomic trajectories, we can sample the interatomic potential of lithium niobate, providing a benchmark for ab initio calculations for the material. Tomography of the energy surface by high-order nonlinear phononics could benefit many aspects of materials research, including the study of classical and quantum phase transitions.

An optical authentication system based on imaging of excitation-selected lanthanide luminescence.

PubMed

Carro-Temboury, Miguel R; Arppe, Riikka; Vosch, Tom; Sørensen, Thomas Just

2018-01-01

Secure data encryption relies heavily on one-way functions, and copy protection relies on features that are difficult to reproduce. We present an optical authentication system based on lanthanide luminescence from physical one-way functions or physical unclonable functions (PUFs). They cannot be reproduced and thus enable unbreakable encryption. Further, PUFs will prevent counterfeiting if tags with unique PUFs are grafted onto products. We have developed an authentication system that comprises a hardware reader, image analysis, and authentication software and physical keys that we demonstrate as an anticounterfeiting system. The physical keys are PUFs made from random patterns of taggants in polymer films on glass that can be imaged following selected excitation of particular lanthanide(III) ions doped into the individual taggants. This form of excitation-selected imaging ensures that by using at least two lanthanide(III) ion dopants, the random patterns cannot be copied, because the excitation selection will fail when using any other emitter. With the developed reader and software, the random patterns are read and digitized, which allows a digital pattern to be stored. This digital pattern or digital key can be used to authenticate the physical key in anticounterfeiting or to encrypt any message. The PUF key was produced with a staggering nominal encoding capacity of 7 3600 . Although the encoding capacity of the realized authentication system reduces to 6 × 10 104 , it is more than sufficient to completely preclude counterfeiting of products.

Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons

DOE PAGES

Soavi, Giancarlo; Dal Conte, Stefano; Manzoni, Cristian; ...

2016-03-17

Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron–hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton–exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ≈250meV, in very goodmore » agreement with theoretical results from quantum Monte Carlo simulations. As a result, these observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics.« less

Multi-function diamond film fiber optic probe and measuring system employing same

DOEpatents

Young, J.P.

1998-11-24

A fused fiber optic probe having a protective cover, a fiber optic probe system, and embodiments thereof for conducting electromagnetic spectral measurements are disclosed. The fused fiber optic probe comprises a probe tip having a specific geometrical configuration, an exciting optical fiber and at least one collection optical fiber fused within a housing, preferably silica, with a protective cover disposed over at least a portion of the probe tip. The specific geometrical configurations in which the probe tip can be shaped include a slanted probe tip with an angle greater than 0{degree}, an inverted cone-shaped probe tip, and a lens head. 9 figs.

A landmark recognition and tracking experiment for flight on the Shuttle/Advanced Technology Laboratory (ATL)

NASA Technical Reports Server (NTRS)

Welch, J. D.

1975-01-01

The preliminary design of an experiment for landmark recognition and tracking from the Shuttle/Advanced Technology Laboratory is described. It makes use of parallel coherent optical processing to perform correlation tests between landmarks observed passively with a telescope and previously made holographic matched filters. The experimental equipment including the optics, the low power laser, the random access file of matched filters and the electro-optical readout device are described. A real time optically excited liquid crystal device is recommended for performing the input non-coherent optical to coherent optical interface function. A development program leading to a flight experiment in 1981 is outlined.

Enhancing Optical Forces in InP-Based Waveguides.

PubMed

Aryaee Panah, Mohammad Esmail; Semenova, Elizaveta S; Lavrinenko, Andrei V

2017-06-08

Cantilever sensors are among the most important microelectromechanical systems (MEMS), which are usually actuated by electrostatic forces or piezoelectric elements. Although well-developed microfabrication technology has made silicon the prevailing material for MEMS, unique properties of other materials are overlooked in this context. Here we investigate optically induced forces exerted upon a semi-insulating InP waveguide suspended above a highly doped InP:Si substrate, in three different regimes: the epsilon-near-zero (ENZ), with excitation of surface plasmon polaritons (SPPs) and phonons excitation. An order of magnitude amplification of the force is observed when light is coupled to SPPs, and three orders of magnitude amplification is achieved in the phonon excitation regime. In the ENZ regime, the force is found to be repulsive and higher than that in a waveguide suspended above a dielectric substrate. Low losses in InP:Si result in a big propagation length. The induced deflection can be detected by measuring the phase change of the light when passing through the waveguide, which enables all-optical functioning, and paves the way towards integration and miniaturization of micro-cantilevers. In addition, tunability of the ENZ and the SPP excitation wavelength ranges, via adjusting the carrier concentration, provides an extra degree of freedom for designing MEMS devices.

Probing molecular potentials with an optical centrifuge.

PubMed

Milner, A A; Korobenko, A; Hepburn, J W; Milner, V

2017-09-28

We use an optical centrifuge to excite coherent rotational wave packets in N 2 O, OCS, and CS 2 molecules with rotational quantum numbers reaching up to J≈465, 690, and 1186, respectively. Time-resolved rotational spectroscopy at such ultra-high levels of rotational excitation can be used as a sensitive tool to probe the molecular potential energy surface at internuclear distances far from their equilibrium values. Significant bond stretching in the centrifuged molecules results in the growing period of the rotational revivals, which are experimentally detected using coherent Raman scattering. We measure the revival period as a function of the centrifuge-induced rotational frequency and compare it with the numerical calculations based on the known Morse-cosine potentials.

Probing molecular potentials with an optical centrifuge

NASA Astrophysics Data System (ADS)

Milner, A. A.; Korobenko, A.; Hepburn, J. W.; Milner, V.

2017-09-01

We use an optical centrifuge to excite coherent rotational wave packets in N2O, OCS, and CS2 molecules with rotational quantum numbers reaching up to J ≈465 , 690, and 1186, respectively. Time-resolved rotational spectroscopy at such ultra-high levels of rotational excitation can be used as a sensitive tool to probe the molecular potential energy surface at internuclear distances far from their equilibrium values. Significant bond stretching in the centrifuged molecules results in the growing period of the rotational revivals, which are experimentally detected using coherent Raman scattering. We measure the revival period as a function of the centrifuge-induced rotational frequency and compare it with the numerical calculations based on the known Morse-cosine potentials.

Dynamic Optical Tuning of Interlayer Interactions in the Transition Metal Dichalcogenides

DOE PAGES

Mannebach, Ehren M.; Nyby, Clara; Ernst, Friederike; ...

2017-11-09

Modulation of weak interlayer interactions between quasi-two-dimensional atomic planes in the transition metal dichalcogenides (TMDCs) provides avenues for tuning their functional properties. Here we show that above-gap optical excitation in the TMDCs leads to an unexpected large-amplitude, ultrafast compressive force between the two-dimensional layers, as probed by in situ measurements of the atomic layer spacing at femtosecond time resolution. We show that this compressive response arises from a dynamic modulation of the interlayer van der Waals interaction and that this represents the dominant light-induced stress at low excitation densities. A simple analytic model predicts the magnitude and carrier density dependencemore » of the measured strains. Furthermore, this work establishes a new method for dynamic, nonequilibrium tuning of correlation-driven dispersive interactions and of the optomechanical functionality of TMDC quasi-two-dimensional materials.« less

First-Principles Studies of the Excited States and Optical Properties of Xanthene Derivative Chromophores

NASA Astrophysics Data System (ADS)

Hamed, Samia; Sharifzadeh, Sahar; Neaton, Jeffrey

2014-03-01

Elucidation of the energy transfer mechanism in natural photosynthetic systems remains an exciting challenge. In particular, biomimetic protein-pigment complexes provide a unique study space in which individual parameters are adjusted and the impact of those changes captured. Here, we compute the excited state properties of a group of xanthene-derivative chromophores to be employed in the construction of new biomimetic light harvesting frameworks. Excitation energies, transition dipoles, and natural transition orbitals for the low-lying singlet and triplet states of these experimentally-relevant chromophores are obtained from first-principles density functional theory. The performance of several exchange-correlation functionals, including an optimally-tuned range-separated hybrid, are evaluated and compared with many body perturbation theory and experiment. Finally, we will discuss the implication of our results for the bottom-up design of new chromophores. This work is supported by the DOE and computational resources are provided by NERSC.

The Study of ( n, d) Reaction Cross Sections for New Evaluated Semi-Empirical Formula Using Optical Model

NASA Astrophysics Data System (ADS)

Bölükdemir, M. H.; Tel, E.; Okuducu, Ş.; Aydın, A.

2009-12-01

Nuclear fusion can be one of the most attractive sources of energy from the viewpoint of safety and minimal environmental impact. The neutron scattering cross sections data have a critical importance on fusion reactor (and in the fusion-fission hybrid) reactors. So, the study of the systematic of ( n, d) etc., reaction cross sections is of great importance in the definition of the excitation function character for reaction taking place on various nuclei at energies up to 20 MeV. In this study, non-elastic cross-sections have been calculated by using optical model for ( n, d) reactions at 14-15 MeV energy. The excitation function character and reaction Q-values depending on the asymmetry term effect for the ( n, d) reaction have been investigated. New coefficients have been obtained and the semi-empirical formulas including optical model non-elastic effects by fitting two parameters for the ( n, d) reaction cross-sections have been suggested. The obtained cross-section formulas with new coefficients have been compared with the available experimental data and discussed.

Photoacoustic microscopy and computed tomography: from bench to bedside

PubMed Central

Wang, Lihong V.; Gao, Liang

2014-01-01

Photoacoustic imaging (PAI) of biological tissue has seen immense growth in the past decade, providing unprecedented spatial resolution and functional information at depths in the optical diffusive regime. PAI uniquely combines the advantages of optical excitation and acoustic detection. The hybrid imaging modality features high sensitivity to optical absorption and wide scalability of spatial resolution with the desired imaging depth. Here we first summarize the fundamental principles underpinning the technology, then highlight its practical implementation, and finally discuss recent advances towards clinical translation. PMID:24905877

Designing Hybrids of Graphene Oxide and Gold Nanoparticles for Nonlinear Optical Response

NASA Astrophysics Data System (ADS)

Yadav, Rajesh Kumar; Aneesh, J.; Sharma, Rituraj; Abhiramnath, P.; Maji, Tuhin Kumar; Omar, Ganesh Ji; Mishra, A. K.; Karmakar, Debjani; Adarsh, K. V.

2018-04-01

Nonlinear optical absorption of light by materials is weak due to its perturbative nature, although a strong nonlinear response is of crucial importance to applications in optical limiting and switching. Here we demonstrate experimentally and theoretically an extremely efficient scheme of excited-state absorption by charge transfer between donor and acceptor materials as a method to enhance the nonlinear absorption by orders of magnitude. With this idea, we demonstrate a strong excited-state absorption (ESA) in reduced graphene oxide that otherwise shows an increased transparency at high fluence and enhancement of ESA by one order of magnitude in graphene oxide by attaching gold nanoparticles (Au NP) in the tandem configuration that acts as an efficient charge-transfer pair when excited at the plasmonic wavelength. To explain the unprecedented enhancement, we develop a five-level rate-equation model based on the charge transfer between the two materials and numerically simulate the results. To understand the correlation of interfacial charge transfer with the concentration and type of the functional ligands attached to the graphene oxide sheet, we investigate the Au-NP—graphene oxide interface with various possible ligand configurations from first-principles calculations. By using the strong ESA of our hybrid materials, we fabricate liquid cell-based high-performance optical limiters with important device parameters better than that of the benchmark optical limiters.

New developments in electronic reference controls for frequency domain optical sensing

NASA Astrophysics Data System (ADS)

Chatni, M. R.; Li, G.; Porterfield, D. M.

2009-05-01

The reference optical path is essential for optical systems which function on the basis of light interference. In the case of frequency domain (FD) fluorescence life-time optrodes, a reference LED is used as a standard for calculating the phase angle. The reference LED is configured so that radiation travels the same length to the detector as that of the fluorescence signal being analyzed. The phase shift, which provides details of fluorescence lifetime, is measured between these two signals - the fluorescence signal and reference LED signal, using a photodetector. We have designed, developed and implemented a FD optrode system without a reference LED. The key requirement of such a system is that phase shifts due to optics at wavelength of fluorescence and electronics have to be calibrated. In the reference-free system, the reference signal comes from the lock-in-amplifier which also drives the excitation LED. The lock-in-amplifier measures the phase shift between the excitation signal and the fluorescence emission signal from the photodetector and is locked at the frequency of modulation of the excitation signal. This insures higher signal to noise ratio and low-noise measurements. The reference-free optrode system removes some constraints on the coupling optics, which help improve the overall performance of the system. After development of electronics, and optimization of coupling optics, the system was calibrated in different oxygen concentration solutions to measure fluorescence intensity and lifetime of the oxygen sensitive dye platinum tetrakis (pentafluorophenyl) porphine (PtTFPP).

Evolution of Excited-State Dynamics in Periodic Au 28, Au 36, Au 44, and Au 52 Nanoclusters

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

Zhou, Meng; Zeng, Chenjie; Sfeir, Matthew Y.

An understanding of the correlation between the atomic structure and optical properties of gold nanoclusters is essential for exploration of their functionalities and applications involving light harvesting and electron transfer. We report the femto-nanosecond excited state dynamics of a periodic series of face-centered cubic (FCC) gold nanoclusters (including Au 28, Au 36, Au 44, and Au 52), which exhibit a set of unique features compared with other similar sized clusters. Molecular-like ultrafast S n → S 1 internal conversions (i.e., radiationless electronic transitions) are observed in the relaxation dynamics of FCC periodic series. Excited-state dynamics with near-HOMO–LUMO gap excitation lacksmore » ultrafast decay component, and only the structural relaxation dominates in the dynamical process, which proves the absence of core–shell relaxation. Interestingly, both the relaxation of the hot carriers and the band-edge carrier recombination become slower as the size increases. The evolution in excited-state properties of this FCC series offers new insight into the structure-dependent properties of metal nanoclusters, which will benefit their optical energy harvesting and photocatalytic applications.« less

Evolution of Excited-State Dynamics in Periodic Au 28, Au 36, Au 44, and Au 52 Nanoclusters

DOE PAGES

Zhou, Meng; Zeng, Chenjie; Sfeir, Matthew Y.; ...

2017-08-10

An understanding of the correlation between the atomic structure and optical properties of gold nanoclusters is essential for exploration of their functionalities and applications involving light harvesting and electron transfer. We report the femto-nanosecond excited state dynamics of a periodic series of face-centered cubic (FCC) gold nanoclusters (including Au 28, Au 36, Au 44, and Au 52), which exhibit a set of unique features compared with other similar sized clusters. Molecular-like ultrafast S n → S 1 internal conversions (i.e., radiationless electronic transitions) are observed in the relaxation dynamics of FCC periodic series. Excited-state dynamics with near-HOMO–LUMO gap excitation lacksmore » ultrafast decay component, and only the structural relaxation dominates in the dynamical process, which proves the absence of core–shell relaxation. Interestingly, both the relaxation of the hot carriers and the band-edge carrier recombination become slower as the size increases. The evolution in excited-state properties of this FCC series offers new insight into the structure-dependent properties of metal nanoclusters, which will benefit their optical energy harvesting and photocatalytic applications.« less

Optical properties of transiently-excited semiconductor hyperbolic metamaterials

DOE PAGES

Campione, Salvatore; Luk, Ting S.; Liu, Sheng; ...

2015-10-02

Ultrafast optical excitation of photocarriers has the potential to transform undoped semiconductor superlattices into semiconductor hyperbolic metamaterials (SHMs). In this paper, we investigate the optical properties associated with such ultrafast topological transitions. We first show reflectance, transmittance, and absorption under TE and TM plane wave incidence. In the unpumped state, the superlattice exhibits a frequency region with high reflectance (>80%) and a region with low reflectance (<1%) for both TE and TM polarizations over a wide range of incidence angles. In contrast, in the photopumped state, the reflectance for both frequencies and polarizations is very low (<1%) for a similarmore » range of angles. Interestingly, this system can function as an all-optical reflection switch on ultrafast timescales. Furthermore, for TM incidence and close to the epsilon-near-zero point of the longitudinal permittivity, directional perfect absorption on ultrafast timescales may also be achieved. Lastly, we discuss the onset of negative refraction in the photopumped state.« less

Optical temperature sensing of NaYbF4: Tm3+@SiO2 core-shell micro-particles induced by infrared excitation.

PubMed

Wang, Xiangfu; Zheng, Jin; Xuan, Yan; Yan, Xiaohong

2013-09-09

NaYbF(4):Tm3+@SiO(2) core-shell micro-particles were synthesized by a hydrothermal method and subsequent ultrasonic coating process. Optical temperature sensing has been observed in NaYbF4: Tm(3+)@SiO(2)core-shell micro-particles with a 980 nm infrared laser as excitation source.The fluorescence intensity ratios, optical temperature sensitivity, and temperature dependent population re-distribution ability from the thermally coupled (1)D(2)/(1)G(4) and (3)F(2) /(3)H(4) levels of the Tm(3+) ion have been analyzed as a function of temperature in the range of 100~700 K in order to check its availability as a optical temperature sensor. A better behavior as a lowtemperature sensor has been obtained with a minimum sensitivity of 5.4 × 10(-4) K(-1) at 430 K. It exhibits temperature induced population re-distribution from (1)D(2) /(1)G(4) thermally coupled levels at higher temperature range.

Comparison of exciplex generation under optical and X-ray excitation

NASA Astrophysics Data System (ADS)

Kipriyanov, A. A.; Melnikov, A. R.; Stass, D. V.; Doktorov, A. B.

2017-09-01

Exciplex generation under optical and X-ray excitation in identical conditions is experimentally compared using a specially chosen model donor-acceptor system, anthracene (electron acceptor) and N,N-dimethylaniline (electron donor) in non-polar solution, and the results are analyzed and interpreted based on analytically calculated luminescence quantum yields. Calculations are performed on the basis of kinetic equations for multistage schemes of bulk exciplex production reaction under optical excitation and combination of bulk and geminate reactions of radical ion pairs under X-ray excitation. These results explain the earlier experimentally found difference in the ratio of the quantum yields of exciplexes and excited electron acceptors (exciplex generation efficiency) and the corresponding change in the exciplex generation efficiency under X-irradiation as compared to the reaction under optical excitation.

Comparison of exciplex generation under optical and X-ray excitation.

PubMed

Kipriyanov, A A; Melnikov, A R; Stass, D V; Doktorov, A B

2017-09-07

Exciplex generation under optical and X-ray excitation in identical conditions is experimentally compared using a specially chosen model donor-acceptor system, anthracene (electron acceptor) and N,N-dimethylaniline (electron donor) in non-polar solution, and the results are analyzed and interpreted based on analytically calculated luminescence quantum yields. Calculations are performed on the basis of kinetic equations for multistage schemes of bulk exciplex production reaction under optical excitation and combination of bulk and geminate reactions of radical ion pairs under X-ray excitation. These results explain the earlier experimentally found difference in the ratio of the quantum yields of exciplexes and excited electron acceptors (exciplex generation efficiency) and the corresponding change in the exciplex generation efficiency under X-irradiation as compared to the reaction under optical excitation.

Relevance of Excitable Media Theory and Retinal Spreading Depression Experiments in Preclinical Pharmacological Research

PubMed Central

V.M, Fernandes de Lima; W, Hanke

2014-01-01

In preclinical neuropharmacological research, molecular, cell-based, and systems using animals are well established. On the tissue level the situation is less comfortable, although during the last decades some effort went into establishing such systems, i.e. using slices of the vertebrate brain together with optical and electrophysiological techniques. However, these methods are neither fast, nor can they be automated or upscaled. By contrast, the chicken retina can be used as a suitable model. It is easy accessible and can be kept alive in vitro for hours up to days. Due to its structure, in addition the retina displays remarkable intrinsic optical signals, which can be easily used in experiments. Also to electrophysiological methods the retina is well accessible. In excitable tissue, to which the brain and the retina belong, propagating excitation waves can be expected, and the spreading depression is such a phenomenon. It has been first observed in the forties of the last century. Later, Martins-Ferreira established it in the chicken retina (retinal spreading depression or RSD). The electrophysiological characteristics of it are identical with those of the cortical SD. The metabolic differences are known and can be taken into account. The experimental advantage of the RSD compared to the cortical SD is the pronounced intrinsic optical signal (IOS) associated with the travelling wave. This is due to the maximum transparency of retinal tissue in the functional state; thus any physiological event will change it markedly and therefore can be easily seen even by naked eye. The theory can explain wave spread in one (action potentials), two (RSDs) and three dimensions (one heart beat). In this review we present the experimental and the excitable media context for the data interpretation using as example the cholinergic pharmacology in relation to functional syndromes. We also discuss the intrinsic optical signal and how to use it in pre-clinical research. PMID:25426010

Laser-induced fluorescence fiber optic probe measurement of oil dilution by fuel

DOEpatents

Parks, II, James E [Knoxville, TN; Partridge, Jr., William P [Oak Ridge, TN

2010-11-23

Apparatus for detecting fuel in oil includes an excitation light source in optical communication with an oil sample for exposing the oil sample to excitation light in order to excite the oil sample from a non-excited state to an excited state and a spectrally selective device in optical communication with the oil sample for detecting light emitted from the oil sample as the oil sample returns from the excited state to a non-excited state to produce spectral indicia that can be analyzed to determine the presence of fuel in the oil sample. A method of detecting fuel in oil includes the steps of exposing a oil sample to excitation light in order to excite the oil sample from a non-excited state to an excited state, as the oil sample returns from the excited state to a non-excited state, detecting light emitted from the oil sample to produce spectral indicia; and analyzing the spectral indicia to determine the presence of fuel in the oil sample.

Spectroscopy of Charged Quantum Dot Molecules

NASA Astrophysics Data System (ADS)

Stinaff, E. A.; Scheibner, M.; Bracker, A. S.; Ponomarev, I. V.; Ware, M. E.; Doty, M. F.; Reinecke, T. L.; Gammon, D.; Korenev, V. L.

2006-03-01

Spins of single charges in quantum dots are attractive for many quantum information and spintronic proposals. Scalable quantum information applications require the ability to entangle and operate on multiple spins in coupled quantum dots (CQDs). To further the understanding of these systems, we present detailed spectroscopic studies of InAs CQDs with control of the discrete electron or hole charging of the system. The optical spectrum reveals a pattern of energy anticrossings and crossings in the photoluminescence as a function of applied electric field. These features can be understood as a superposition of charge and spin configurations of the two dots and represent clear signatures of quantum mechanical coupling. The molecular resonance leading to these anticrossings is achieved at different electric fields for the optically excited (trion) states and the ground (hole) states allowing for the possibility of using the excited states for optically induced coupling of the qubits.

Exact stochastic unraveling of an optical coherence dynamics by cumulant expansion

NASA Astrophysics Data System (ADS)

Olšina, Jan; Kramer, Tobias; Kreisbeck, Christoph; Mančal, Tomáš

2014-10-01

A numerically exact Monte Carlo scheme for calculation of open quantum system dynamics is proposed and implemented. The method consists of a Monte Carlo summation of a perturbation expansion in terms of trajectories in Liouville phase-space with respect to the coupling between the excited states of the molecule. The trajectories are weighted by a complex decoherence factor based on the second-order cumulant expansion of the environmental evolution. The method can be used with an arbitrary environment characterized by a general correlation function and arbitrary coupling strength. It is formally exact for harmonic environments, and it can be used with arbitrary temperature. Time evolution of an optically excited Frenkel exciton dimer representing a molecular exciton interacting with a charge transfer state is calculated by the proposed method. We calculate the evolution of the optical coherence elements of the density matrix and linear absorption spectrum, and compare them with the predictions of standard simulation methods.

Two-color field enhancement at an STM junction for spatiotemporally resolved photoemission

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

Meng, Xiang; Jin, Wencan; Yang, Hao

Here, we report measurements and numerical simulations of ultrafast laser-excited carrier flow across a scanning tunneling microscope (STM) junction. The current from a nanoscopic tungsten tip across a ~1 nm vacuum gap to a silver surface is driven by a two-color excitation scheme that uses an optical delay-modulation technique to extract the two-color signal from background contributions. The role of optical field enhancements in driving the current is investigated using density functional theory and full three-dimensional finite-difference time-domain computations. We find that simulated field-enhanced two-photon photoemission (2PPE) currents are in excellent agreement with the observed exponential decay of the two-colormore » photoexcited current with increasing tip–surface separation, as well as its optical-delay dependence. The results suggest an approach to 2PPE with simultaneous subpicosecond temporal and nanometer spatial resolution.« less

Optical sensors based on photonic crystal: a new route

NASA Astrophysics Data System (ADS)

Romano, S.; Torino, S.; Coppola, G.; Cabrini, S.; Mocella, V.

2017-05-01

The realization of miniaturized devices able to accumulate a higher number of information in a smallest volume is a challenge of the technological development. This trend increases the request of high sensitivity and selectivity sensors which can be integrated in microsystems. In this landscape, optical sensors based on photonic crystal technology can be an appealing solution. Here, a new refractive index sensor device, based on the bound states in the continuum (BIC) resonance shift excited in a photonic crystal membrane, is presented. A microfluidic cell was used to control the injection of fluids with different refractive indices over the photonic crystal surface. The shift of very high Q-factor resonances excited into the photonic crystal open cavity was monitored as a function of the refractive index n of the test liquid. The excellent stability we found and the minimal, loss-free optical equipment requirement, provide a new route for achieving high performance in sensing applications.

Two-color field enhancement at an STM junction for spatiotemporally resolved photoemission

DOE PAGES

Meng, Xiang; Jin, Wencan; Yang, Hao; ...

2017-06-30

Here, we report measurements and numerical simulations of ultrafast laser-excited carrier flow across a scanning tunneling microscope (STM) junction. The current from a nanoscopic tungsten tip across a ~1 nm vacuum gap to a silver surface is driven by a two-color excitation scheme that uses an optical delay-modulation technique to extract the two-color signal from background contributions. The role of optical field enhancements in driving the current is investigated using density functional theory and full three-dimensional finite-difference time-domain computations. We find that simulated field-enhanced two-photon photoemission (2PPE) currents are in excellent agreement with the observed exponential decay of the two-colormore » photoexcited current with increasing tip–surface separation, as well as its optical-delay dependence. The results suggest an approach to 2PPE with simultaneous subpicosecond temporal and nanometer spatial resolution.« less

Genetically Targeted All-Optical Electrophysiology with a Transgenic Cre-Dependent Optopatch Mouse

PubMed Central

Lou, Shan; Adam, Yoav; Weinstein, Eli N.; Williams, Erika; Williams, Katherine; Parot, Vicente; Kavokine, Nikita; Liberles, Stephen; Madisen, Linda; Zeng, Hongkui

2016-01-01

Recent advances in optogenetics have enabled simultaneous optical perturbation and optical readout of membrane potential in diverse cell types. Here, we develop and characterize a Cre-dependent transgenic Optopatch2 mouse line that we call Floxopatch. The animals expressed a blue-shifted channelrhodopsin, CheRiff, and a near infrared Archaerhodopsin-derived voltage indicator, QuasAr2, via targeted knock-in at the rosa26 locus. In Optopatch-expressing animals, we tested for overall health, genetically targeted expression, and function of the optogenetic components. In offspring of Floxopatch mice crossed with a variety of Cre driver lines, we observed spontaneous and optically evoked activity in vitro in acute brain slices and in vivo in somatosensory ganglia. Cell-type-specific expression allowed classification and characterization of neuronal subtypes based on their firing patterns. The Floxopatch mouse line is a useful tool for fast and sensitive characterization of neural activity in genetically specified cell types in intact tissue. SIGNIFICANCE STATEMENT Optical recordings of neural activity offer the promise of rapid and spatially resolved mapping of neural function. Calcium imaging has been widely applied in this mode, but is insensitive to the details of action potential waveforms and subthreshold events. Simultaneous optical perturbation and optical readout of single-cell electrical activity (“Optopatch”) has been demonstrated in cultured neurons and in organotypic brain slices, but not in acute brain slices or in vivo. Here, we describe a transgenic mouse in which expression of Optopatch constructs is controlled by the Cre-recombinase enzyme. This animal enables fast and robust optical measurements of single-cell electrical excitability in acute brain slices and in somatosensory ganglia in vivo, opening the door to rapid optical mapping of neuronal excitability. PMID:27798186

Optical signatures of coupled quantum dots.

PubMed

Stinaff, E A; Scheibner, M; Bracker, A S; Ponomarev, I V; Korenev, V L; Ware, M E; Doty, M F; Reinecke, T L; Gammon, D

2006-02-03

An asymmetric pair of coupled InAs quantum dots is tuned into resonance by applying an electric field so that a single hole forms a coherent molecular wave function. The optical spectrum shows a rich pattern of level anticrossings and crossings that can be understood as a superposition of charge and spin configurations of the two dots. Coulomb interactions shift the molecular resonance of the optically excited state (charged exciton) with respect to the ground state (single charge), enabling light-induced coupling of the quantum dots. This result demonstrates the possibility of optically coupling quantum dots for application in quantum information processing.

Optical Signatures of Coupled Quantum Dots

NASA Astrophysics Data System (ADS)

Stinaff, E. A.; Scheibner, M.; Bracker, A. S.; Ponomarev, I. V.; Korenev, V. L.; Ware, M. E.; Doty, M. F.; Reinecke, T. L.; Gammon, D.

2006-02-01

An asymmetric pair of coupled InAs quantum dots is tuned into resonance by applying an electric field so that a single hole forms a coherent molecular wave function. The optical spectrum shows a rich pattern of level anticrossings and crossings that can be understood as a superposition of charge and spin configurations of the two dots. Coulomb interactions shift the molecular resonance of the optically excited state (charged exciton) with respect to the ground state (single charge), enabling light-induced coupling of the quantum dots. This result demonstrates the possibility of optically coupling quantum dots for application in quantum information processing.

Mode-selective mapping and control of vectorial nonlinear-optical processes in multimode photonic-crystal fibers.

PubMed

Hu, Ming-Lie; Wang, Ching-Yue; Song, You-Jian; Li, Yan-Feng; Chai, Lu; Serebryannikov, Evgenii; Zheltikov, Aleksei

2006-02-06

We demonstrate an experimental technique that allows a mapping of vectorial nonlinear-optical processes in multimode photonic-crystal fibers (PCFs). Spatial and polarization modes of PCFs are selectively excited in this technique by varying the tilt angle of the input beam and rotating the polarization of the input field. Intensity spectra of the PCF output plotted as a function of the input field power and polarization then yield mode-resolved maps of nonlinear-optical interactions in multimode PCFs, facilitating the analysis and control of nonlinear-optical transformations of ultrashort laser pulses in such fibers.

High speed all optical logic gates based on quantum dot semiconductor optical amplifiers.

PubMed

Ma, Shaozhen; Chen, Zhe; Sun, Hongzhi; Dutta, Niloy K

2010-03-29

A scheme to realize all-optical Boolean logic functions AND, XOR and NOT using semiconductor optical amplifiers with quantum-dot active layers is studied. nonlinear dynamics including carrier heating and spectral hole-burning are taken into account together with the rate equations scheme. Results show with QD excited state and wetting layer serving as dual-reservoir of carriers, as well as the ultra fast carrier relaxation of the QD device, this scheme is suitable for high speed Boolean logic operations. Logic operation can be carried out up to speed of 250 Gb/s.

Laser inhibited diffusion in rhodamine-ethanol solutions

NASA Technical Reports Server (NTRS)

Lawandy, N. M.; Fuhr, P. L.; Robinson, D. W.

1981-01-01

The diffusion of rhodamine-6G dye in ethanol is observed to be inhibited by optical pumping by a cadmium laser. The diffusion process is observed as a function of the solution temperature. The relative difference in diffusion coefficients with and without optical pumping is calculated. The effect is interpreted as being due to a stronger solvent-dye interaction in the first excited singlet state of rhodamine-6G.

Photon Antibunching in the Fluorescence of a Single Dye Molecule Trapped in a Solid

DTIC Science & Technology

1992-06-08

number) FIELD GROUP SUB-GROUP single-molecule spectroscopy in solids, photon antibunching, quantum-optics, nonclassical effects pentacene in p-terphenyl...emitted by an optically pumped single molecule of pentacene In a p-terphenyl host has been Investigated at short times. The correlation function...excitation tcclnique, certain individual pentacene impurity molecules in a p-terphenyl crystal 11 were observed to spectrally diffuse, i.e. their absorption

Semiempirical modeling of Ag nanoclusters: New parameters for optical property studies enable determination of double excitation contributions to plasmonic excitation

DOE PAGES

Gieseking, Rebecca L.; Ratner, Mark A.; Schatz, George C.

2016-06-03

Quantum mechanical studies of Ag nanoclusters have shown that plasmonic behavior can be modeled in terms of excited states where collectivity among single excitations leads to strong absorption. However, new computational approaches are needed to provide understanding of plasmonic excitations beyond the single-excitation level. We show that semiempirical INDO/CI approaches with appropriately selected parameters reproduce the TD-DFT optical spectra of various closed-shell Ag clusters. The plasmon-like states with strong optical absorption comprise linear combinations of many singly excited configurations that contribute additively to the transition dipole moment, whereas all other excited states show significant cancellation among the contributions to themore » transition dipole moment. The computational efficiency of this approach allows us to investigate the role of double excitations at the INDO/SDCI level. The Ag cluster ground states are stabilized by slight mixing with doubly excited configurations, but the plasmonic states generally retain largely singly excited character. The consideration of double excitations in all cases improves the agreement of the INDO/CI absorption spectra with TD-DFT, suggesting that the SDCI calculation effectively captures some of the ground-state correlation implicit in DFT. Furthermore, these results provide the first evidence to support the commonly used assumption that single excitations are in many cases sufficient to describe the optical spectra of plasmonic excitations quantum mechanically.« less

Direct detection of time-resolved Rabi oscillations in a single quantum dot via resonance fluorescence

NASA Astrophysics Data System (ADS)

Schaibley, J. R.; Burgers, A. P.; McCracken, G. A.; Steel, D. G.; Bracker, A. S.; Gammon, D.; Sham, L. J.

2013-03-01

Optical Rabi oscillations are coherent population oscillations of a two-level system coupled by an electric dipole transition when driven by a strong nearly resonant optical field. In quantum dot structures, these measurements have typically been performed as a function of the total pulse area ∫Ω0(t)dt where the pulse area varies as a function of Rabi frequency. Here, we report direct detection of the time-resolved coherent transient response of the resonance fluorescence to measure the time evolution of the optical Rabi oscillations in a single charged InAs quantum dot. We extract a decoherence rate consistent with the limit from the excited state lifetime.

FUNDUS AUTOFLUORESCENCE IN RUBELLA RETINOPATHY: Correlation With Photoreceptor Structure and Function.

PubMed

Bukowska, Danuta M; Wan, Sue Ling; Chew, Avenell L; Chelva, Enid; Tang, Ivy; Mackey, David A; Chen, Fred K

2017-01-01

To illustrate altered fundus autofluorescence in rubella retinopathy and to investigate their relationships with photoreceptor structure and function using multimodal imaging. The authors report four cases of rubella retinopathy aged 8, 33, 42, and 50 years. All patients had dilated clinical fundus examination; wide-field color photography; blue, green, and near-infrared autofluorescence imaging and spectral domain optical coherence tomography. Two patients also underwent microperimetry and adaptive optics imaging. En face optical coherence tomography, cone mosaic, and microperimetry were coregistered with autofluorescence images. The authors explored the structure-function correlation. All four patients had a "salt-and-pepper" appearance on dilated fundus examination and wide-field color photography. There were variable-sized patches of hypoautofluorescence on both blue and near-infrared excitation in all four patients. Wave-guiding cones were visible and retinal sensitivity was intact over these regions. There was no correlation between hypoautofluorescence and regions of attenuated ellipsoid and interdigitation zones. Hyperautofluorescent lesions were also noted and some of these were pseudo-vitelliform lesions. Patchy hypoautofluorescence on near-infrared excitation can be a feature of rubella retinopathy. This may be due to abnormal melanin production or loss of melanin within retinal pigment epithelium cells harboring persistent rubella virus infection. Preservation of the ellipsoid zone, wave-guiding cones, and retinal sensitivity within hypoautofluorescent lesions suggest that these retinal pigment epithelium changes have only mild impact on photoreceptor cell function.

Pulsed laser versus electrical energy for peripheral nerve stimulation

PubMed Central

Wells, Jonathon; Konrad, Peter; Kao, Chris; Jansen, E. Duco; Mahadevan-Jansen, Anita

2010-01-01

Transient optical neural stimulation has previously been shown to elicit highly controlled, artifact-free potentials within the nervous system in a non-contact fashion without resulting in damage to tissue. This paper presents the physiologic validity of elicited nerve and muscle potentials from pulsed laser induced stimulation of the peripheral nerve in a comparative study with the standard method of electrically evoked potentials. Herein, the fundamental physical properties underlying the two techniques are contrasted. Key laser parameters for efficient optical stimulation of the peripheral nerve are detailed. Strength response curves are shown to be linear for each stimulation modality, although fewer axons can be recruited with optically evoked potentials. Results compare the relative transient energy requirements for stimulation using each technique and demonstrate that optical methods can selectively excite functional nerve stimulation. Adjacent stimulation and recording of compound nerve potentials in their entirety from optical and electrical stimulation are presented, with optical responses shown to be free of any stimulation artifact. Thus, use of a pulsed laser exhibits some advantages when compared to standard electrical means for excitation of muscle potentials in the peripheral nerve in the research domain and possibly for clinical diagnostics in the future. PMID:17537515

Access to long-term optical memories using photon echoes retrieved from electron spins in semiconductor quantum wells

NASA Astrophysics Data System (ADS)

Poltavtsev, S. V.; Langer, L.; Yugova, I. A.; Salewski, M.; Kapitonov, Y. V.; Yakovlev, D. R.; Karczewski, G.; Wojtowicz, T.; Akimov, I. A.; Bayer, M.

2016-10-01

We use spontaneous (two-pulse) and stimulated (three-pulse) photon echoes for studying the coherent evolution of optically excited ensemble of trions which are localized in semiconductor CdTe/CdMgTe quantum well. Application of transverse magnetic field leads to the Larmor precession of the resident electron spins, which shuffles optically induced polarization between optically accessible and inaccessible states. This results in several spectacular phenomena. First, magnetic field induces oscillations of spontaneous photon echo amplitude. Second, in three-pulse excitation scheme, the photon echo decay is extended by several orders of magnitude. In this study, short-lived optical excitation which is created by the first pulse is coherently transferred into a long-lived electron spin state using the second optical pulse. This coherent spin state of electron ensemble persists much longer than any optical excitation in the system, preserving information on initial optical field, which can be retrieved as a photon echo by means of third optical pulse.

Ultrafast optical excitation of magnetic skyrmions

NASA Astrophysics Data System (ADS)

Ogawa, N.; Seki, S.; Tokura, Y.

2015-04-01

Magnetic skyrmions in an insulating chiral magnet Cu2OSeO3 were studied by all-optical spin wave spectroscopy. The spins in the conical and skyrmion phases were excited by the impulsive magnetic field from the inverse-Faraday effect, and resultant spin dynamics were detected by using time-resolved magneto-optics. Clear dispersions of the helimagnon were observed, which is accompanied by a distinct transition into the skyrmion phase, by sweeping temperature and magnetic field. In addition to the collective excitations of skyrmions, i.e., rotation and breathing modes, several spin precession modes were identified, which would be specific to optical excitation. The ultrafast, nonthermal, and local excitation of the spin systems by photons would lead to the efficient manipulation of nano-magnetic structures.

Holograms for power-efficient excitation of optical surface waves

NASA Astrophysics Data System (ADS)

Ignatov, Anton I.; Merzlikin, Alexander M.

2018-02-01

A method for effective excitation of optical surface waves based on holography principles has been proposed. For a particular example of excitation of a plasmonic wave in a dielectric layer on metal the efficiency of proposed volume holograms in the dielectric layer has been analyzed in comparison with optimized periodic gratings in the dielectric layer. Conditions when the holograms are considerably more efficient than the gratings have been found out. In addition, holograms recorded in two iterations have been proposed and studied. Such holograms are substantially more efficient than the optimized periodic gratings for all incidence angles of an exciting Gaussian beam. The proposed method is universal: it can be extended for efficient excitation of different types of optical surface waves and optical waveguide modes.

Nonlinear Optical Properties and Applications of Polydiacetylene

NASA Technical Reports Server (NTRS)

Abdeldayem, Hossin; Paley, Mark S.; Witherow, William K.; Frazier, Donald O.

2000-01-01

Recently, we have demonstrated a picosecond all-optical switch, which also functions as a partial all-optical NAND logic gate using a novel polydiacetylene that is synthesized in our laboratory. The nonlinear optical properties of the polydiacetylene material are measured using the Z-scan technique. A theoretical model based on a three level system is investigated and the rate equations of the system are solved. The theoretical calculations are proven to match nicely with the experimental results. The absorption cross-sections for both the first and higher excited states are estimated. The analyses also show that the material suffers a photochemical change beyond a certain level of the laser power and its physical properties suffer radical changes. These changes are the cause for the partial NAND gate function and the switching mechanism.

Local field effects in the energy transfer between a chromophore and a carbon nanotube: a single-nanocompound investigation.

PubMed

Roquelet, Cyrielle; Vialla, Fabien; Diederichs, Carole; Roussignol, Philippe; Delalande, Claude; Deleporte, Emmanuelle; Lauret, Jean-Sébastien; Voisin, Christophe

2012-10-23

Energy transfer in noncovalently bound porphyrin/carbon nanotube compounds is investigated at the single-nanocompound scale. Excitation spectroscopy of the luminescence of the nanotube shows two resonances arising from intrinsic excitation of the nanotube and from energy transfer from the porphyrin. Polarization diagrams show that both resonances are highly anisotropic, with a preferred direction along the tube axis. The energy transfer is thus strongly anisotropic despite the almost isotropic absorption of porphyrins. We account for this result by local field effects induced by the large optical polarizability of nanotubes. We show that the local field correction extends over several nanometers outside the nanotubes and drives the overall optical response of functionalized nanotubes.

Excitation of multipolar surface plasmon resonance in plasmonic nanoparticles by complex accelerating beams

NASA Astrophysics Data System (ADS)

Yang, Yang; Li, Jiafang; Li, Zhi-Yuan; Chen, Yue-Gang

2015-07-01

In this paper, through a vector-spherical harmonics approach, we investigate the optical spectra of plasmonic Au nanoparticles excited by two special accelerating beams: a non-paraxial Airy beam and a Bessel beam. We systematically analyze the impacts of the beam profile, phase, and helical wave front of the electromagnetic fields on the optical spectrum and the excitation of the surface plasmon resonance (SPR). We find that the high-order phase in the Airy beam would result in strong plasmonic oscillations in the optical spectra, while the cone angle and orbital angular momentum carried by the Bessel beam could be employed to engineer the plasmon modes excited in Au nanoparticles. Furthermore, the optical spectrum excited by a combined Airy-Bessel-Gauss beam is discussed. The study could help to deeply explore new ways to manipulate SPR in metal nanoparticles via the wave front engineering of optical beams for enhancing light-matter interaction and optical sensing performance.

Final Technical Report for DE-SC0001878 [Theory and Simulation of Defects in Oxide Materials

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

Chelikowsky, James R.

2014-04-14

We explored a wide variety of oxide materials and related problems, including materials at the nanoscale and generic problems associated with oxide materials such as the development of more efficient computational tools to examine these materials. We developed and implemented methods to understand the optical and structural properties of oxides. For ground state properties, our work is predominantly based on pseudopotentials and density functional theory (DFT), including new functionals and going beyond the local density approximation (LDA): LDA+U. To study excited state properties (quasiparticle and optical excitations), we use time dependent density functional theory, the GW approach, and GW plusmore » Bethe-Salpeter equation (GW-BSE) methods based on a many-body Green function approaches. Our work focused on the structural, electronic, optical and magnetic properties of defects (such as oxygen vacancies) in hafnium oxide, titanium oxide (both bulk and clusters) and related materials. We calculated the quasiparticle defect states and charge transition levels of oxygen vacancies in monoclinic hafnia. we presented a milestone G0W0 study of two of the crystalline phases of dye-sensitized TiO{sub 2} clusters. We employed hybrid density functional theory to examine the electronic structure of sexithiophene/ZnO interfaces. To identify the possible effect of epitaxial strain on stabilization of the ferromagnetic state of LaCoO{sub 3} (LCO), we compare the total energy of the magnetic and nonmagnetic states of the strained theoretical bulk structure.« less

Light, Molecules, Action: Broadband UV-visible transient absorption studies of excited state dynamics in photoactive molecules

NASA Astrophysics Data System (ADS)

Sension, Roseanne

2015-03-01

Broadband UV-visible transient absorption spectroscopy provides a powerful tool for the investigation of the dynamics of electronically excited molecules in the condensed phase. It is now possible to obtain transient spectra on a routine basis spanning the range from <300 nm to >800 nm with femtosecond time resolution. We have used this method to study the excited state dynamics and internal conversion of a range of molecular systems with potential application as optically powered molecular devices. The cyclohexadiene ring-opening reaction is the basis of a class of important optical switches and of the biological synthesis of previtamin D3. The ring-opening reaction is ultrafast, occurring on a picosecond to subpicosecond times scale depending on the substituents around the ring. These have a significant influence on the dynamics and electronic structure of the electronically excited molecule. The results of a series of transient absorption studies as a function of chromophore substitution and environment will be presented. The cis-trans isomerization of polyene molecules, especially substituted stilbenes, provides another important class of functional molecular transformations. Again the excited state dynamics can be ultrafast with photochemistry controlled by details of the curve crossings and conical intersections. Finally the photochemistry of the even more complex set of cobalamin chromophores with a photoalabile C-Co bond has been proposed as a tool for spatio-temporal control of molecule delivery including drug delivery. Broadband transient absorption spectroscopy has been used to investigate the ultrafast electronic dynamics of a range of cobalamin compounds with comparison to detailed theoretical calculations. The results of these studies will be presented.

Advanced synchronous luminescence imaging for chemical and medical diagnostics

DOEpatents

Vo-Dinh, Tuan

2006-09-05

A diagnostic method and associated system includes the steps of exposing at least one sample location with excitation radiation through a single optical waveguide or a single optical waveguide bundle, wherein the sample emits emission radiation in response to the excitation radiation. The same single optical waveguide or the single optical waveguide bundle receives at least a portion of the emission radiation from the sample, thus providing co-registration of the excitation radiation and the emission radiation. The wavelength of the excitation radiation and emission radiation is synchronously scanned to produce a spectrum upon which an image can be formed. An increased emission signal is generated by the enhanced overlap of the excitation and emission focal volumes provided by co-registration of the excitation and emission signals thus increasing the sensitivity as well as decreasing the exposure time necessary to obtain an image.

Advanced multiphoton methods for in vitro and in vivo functional imaging of mouse retinal neurons (Conference Presentation)

NASA Astrophysics Data System (ADS)

Cohen, Noam; Schejter, Adi; Farah, Nairouz; Shoham, Shy

2016-03-01

Studying the responses of retinal ganglion cell (RGC) populations has major significance in vision research. Multiphoton imaging of optogenetic probes has recently become the leading approach for visualizing neural populations and has specific advantages for imaging retinal activity during visual stimulation, because it leads to reduced direct photoreceptor excitation. However, multiphoton retinal activity imaging is not straightforward: point-by-point scanning leads to repeated neural excitation while optical access through the rodent eye in vivo has proven highly challenging. Here, we present two enabling optical designs for multiphoton imaging of responses to visual stimuli in mouse retinas expressing calcium indicators. First, we present an imaging solution based on Scanning Line Temporal Focusing (SLITE) for rapidly imaging neuronal activity in vitro. In this design, we scan a temporally focused line rather than a point, increasing the scan speed and reducing the impact of repeated excitation, while maintaining high optical sectioning. Second, we present the first in vivo demonstration of two-photon imaging of RGC activity in the mouse retina. To obtain these cellular resolution recordings we integrated an illumination path into a correction-free imaging system designed using an optical model of the mouse eye. This system can image at multiple depths using an electronically tunable lens integrated into its optical path. The new optical designs presented here overcome a number of outstanding obstacles, allowing the study of rapid calcium- and potentially even voltage-indicator signals both in vitro and in vivo, thereby bringing us a step closer toward distributed monitoring of action potentials.

All optical experimental design for neuron excitation, inhibition, and action potential detection

NASA Astrophysics Data System (ADS)

Walsh, Alex J.; Tolstykh, Gleb; Martens, Stacey; Sedelnikova, Anna; Ibey, Bennett L.; Beier, Hope T.

2016-03-01

Recently, infrared light has been shown to both stimulate and inhibit excitatory cells. However, studies of infrared light for excitatory cell inhibition have been constrained by the use of invasive and cumbersome electrodes for cell excitation and action potential recording. Here, we present an all optical experimental design for neuronal excitation, inhibition, and action potential detection. Primary rat neurons were transfected with plasmids containing the light sensitive ion channel CheRiff. CheRiff has a peak excitation around 450 nm, allowing excitation of transfected neurons with pulsed blue light. Additionally, primary neurons were transfected with QuasAr2, a fast and sensitive fluorescent voltage indicator. QuasAr2 is excited with yellow or red light and therefore does not spectrally overlap CheRiff, enabling imaging and action potential activation, simultaneously. Using an optic fiber, neurons were exposed to blue light sequentially to generate controlled action potentials. A second optic fiber delivered a single pulse of 1869nm light to the neuron causing inhibition of the evoked action potentials (by the blue light). When used in concert, these optical techniques enable electrode free neuron excitation, inhibition, and action potential recording, allowing research into neuronal behaviors with high spatial fidelity.

Light and ultrasound activated microbubbles around gold nanorods for photoacoustic microsurgery

NASA Astrophysics Data System (ADS)

Cavigli, Lucia; Centi, Sonia; Lai, Sarah; Borri, Claudia; Micheletti, Filippo; Tortoli, Paolo; Panettieri, Ilaria; Streit, Ingolf; Rossi, Francesca; Ratto, Fulvio; Pini, Roberto

2017-07-01

Photoacoustic imaging and microsurgery have recently attracted attention for applications in oncology. Here, we present a versatile set-up to trigger vapor microbubbles around plasmonic nanoparticles by a combined light-ultrasound excitation. This system enables the detection and parametrization of bubbles as a function of several variables, such us optical fluence, ultrasound intensity, nanoparticles concentration, thus providing useful directions to the development of new strategies for treatments based on optical cavitation.

Impact of wavefront distortion and scattering on 2-photon microscopy in mammalian brain tissue

PubMed Central

Chaigneau, Emmanuelle; Wright, Amanda J.; Poland, Simon P.; Girkin, John M.; Silver, R. Angus

2011-01-01

Two-photon (2P) microscopy is widely used in neuroscience, but the optical properties of brain tissue are poorly understood. We have investigated the effect of brain tissue on the 2P point spread function (PSF2P) by imaging fluorescent beads through living cortical slices. By combining this with measurements of the mean free path of the excitation light, adaptive optics and vector-based modeling that includes phase modulation and scattering, we show that tissue-induced wavefront distortions are the main determinant of enlargement and distortion of the PSF2P at intermediate imaging depths. Furthermore, they generate surrounding lobes that contain more than half of the 2P excitation. These effects reduce the resolution of fine structures and contrast and they, together with scattering, limit 2P excitation. Our results disentangle the contributions of scattering and wavefront distortion in shaping the cortical PSF2P, thereby providing a basis for improved 2P microscopy. PMID:22109156

Selective far-field addressing of coupled quantum dots in a plasmonic nanocavity.

PubMed

Tang, Jianwei; Xia, Juan; Fang, Maodong; Bao, Fanglin; Cao, Guanjun; Shen, Jianqi; Evans, Julian; He, Sailing

2018-04-27

Plasmon-emitter hybrid nanocavity systems exhibit strong plasmon-exciton interactions at the single-emitter level, showing great potential as testbeds and building blocks for quantum optics and informatics. However, reported experiments involve only one addressable emitting site, which limits their relevance for many fundamental questions and devices involving interactions among emitters. Here we open up this critical degree of freedom by demonstrating selective far-field excitation and detection of two coupled quantum dot emitters in a U-shaped gold nanostructure. The gold nanostructure functions as a nanocavity to enhance emitter interactions and a nanoantenna to make the emitters selectively excitable and detectable. When we selectively excite or detect either emitter, we observe photon emission predominantly from the target emitter with up to 132-fold Purcell-enhanced emission rate, indicating individual addressability and strong plasmon-exciton interactions. Our work represents a step towards a broad class of plasmonic devices that will enable faster, more compact optics, communication and computation.

A review of materials engineering in silicon-based optical fibres

NASA Astrophysics Data System (ADS)

Healy, Noel; Gibson, Ursula; Peacock, Anna C.

2018-02-01

Semiconductor optical fibre technologies have grown rapidly in the last decade and there are now a range of production and post-processing techniques that allow for a vast degree of control over the core material's optoelectronic properties. These methodologies and the unique optical fibre geometry provide an exciting platform for materials engineering and fibres can now be produced with single crystal cores, low optical losses, tunable strain, and inscribable phase composition. This review discusses the state-of-the-art regarding the production of silicon optical fibres in amorphous and crystalline form and then looks at the post-processing techniques and the improved material quality and new functionality that they afford.

Quasi-particle energies and optical excitations of hydrogenated and fluorinated germanene.

PubMed

Shu, Huabing; Li, Yunhai; Wang, Shudong; Wang, Jinlan

2015-02-14

Using density functional theory, the G0W0 method and Bethe-Salpeter equation calculations, we systematically explore the structural, electronic and optical properties of hydrogenated and fluorinated germanene. The hydrogenated/fluorinated germanene tends to form chair and zigzag-line configurations and its electronic and optical properties show close geometry dependence. The chair hydrogenated/fluorinated and zigzag-line fluorinated germanene are direct band-gap semiconductors, while the zigzag-line hydrogenated germanene owns an indirect band-gap. Moreover, the quasi-particle corrections are significant and strong excitonic effects with large exciton binding energies are observed. Moreover, the zigzag-line hydrogenated/fluorinated germanene shows highly anisotropic optical responses, which may be used as a good optical linear polarizer.

Direct Observation of Optical Field Phase Carving in the Vicinity of Plasmonic Metasurfaces.

PubMed

Dagens, B; Février, M; Gogol, P; Blaize, S; Apuzzo, A; Magno, G; Mégy, R; Lerondel, G

2016-07-13

Plasmonic surfaces are mainly used for their optical intensity concentration properties that allow for enhancement of physical interaction like in nonlinear optics, optical sensors, or tweezers. Phase response in plasmonic resonances can also play a major role, especially in a periodic assembly of plasmonic resonators like metasurfaces. Here we show that localized surface plasmons collectively excited by a guided mode in a metallic nanostructure periodic chain present nonmonotonous phase variation along the 1D metasurface, resulting from both selective Bloch mode coupling and dipolar coupling. As shown by near-field measurements, the phase profile of the highly concentrated optical field is carved out in the vicinity of the metallic metasurface, paving the way to unusual local optical functions.

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

Bičiūnas, A.; Arlauskas, A.; Adamonis, J.

We report on terahertz (THz) emission from tellurium crystal surfaces excited by femtosecond optical pulses. Measurements were performed on three differently cut Te samples and with different wavelength optical excitation pulses. THz pulse amplitude dependences on the azimuthal angle measured at various excitation wavelengths have evidenced that three different mechanisms are responsible for THz generation in tellurium: second order nonlinear optical rectification effect, dominating at lower excitation photon energies, as well as transverse and ordinary photo-Dember effects, which emerge at energies larger than 0.9 eV. The shapes of the azimuthal angle dependences were also explained by theoretical model.

Looking for Speed!! Go Optical Ultra-Fast Photonic Logic Gates for the Future Optical Communication and Computing

NASA Technical Reports Server (NTRS)

Abdeldayem, Hossin; Frazier, Donald O.; Penn, Benjamin; Paley, Mark S.

2003-01-01

Recently, we developed two ultra-fast all-optical switches in the nanosecond and picosecond regimes. The picosecond switch is made of a polydiacetylene thin film coated on the interior wall of a hollow capillary of approximately 50 micron diameter by a photo-polymerization process. In the setup a picosecond Nd:YAG laser at 10 Hz and at 532 nm with a pulse duration of approximately 40 ps was sent collinearly along a cw He-Ne laser beam and both were waveguided through the hollow capillary. The setup functioned as an Exclusive OR gate. On the other hand, the material used in the nanosecond switch is a phthalocyanine thin film, deposited on a glass substrate by a vapor deposition technique. In the setup a nanosecond, 10 Hz, Nd:YAG laser of 8 ns pulse duration was sent collinearly along a cw He-Ne laser beam and both were wave-guided through the phthalocyanine thin film. The setup in this case functioned as an all-optical AND logic gate. The characteristic table of the ExOR gate in polydiacetylene film was attributed to an excited state absorption process, while that of the AND gate was attributed to a saturation process of the first excited state. Both mechanisms were thoroughly investigated theoretically and found to agree remarkably well with the experimental results. An all-optical inverter gate has been designed but has not yet been demonstrated. The combination of all these three gates form the foundation for building all the necessary gates needed to build a prototype of an all-optical system.

Excitability and optical pulse generation in semiconductor lasers driven by resonant tunneling diode photo-detectors.

PubMed

Romeira, Bruno; Javaloyes, Julien; Ironside, Charles N; Figueiredo, José M L; Balle, Salvador; Piro, Oreste

2013-09-09

We demonstrate, experimentally and theoretically, excitable nanosecond optical pulses in optoelectronic integrated circuits operating at telecommunication wavelengths (1550 nm) comprising a nanoscale double barrier quantum well resonant tunneling diode (RTD) photo-detector driving a laser diode (LD). When perturbed either electrically or optically by an input signal above a certain threshold, the optoelectronic circuit generates short electrical and optical excitable pulses mimicking the spiking behavior of biological neurons. Interestingly, the asymmetric nonlinear characteristic of the RTD-LD allows for two different regimes where one obtain either single pulses or a burst of multiple pulses. The high-speed excitable response capabilities are promising for neurally inspired information applications in photonics.

ZnO nanotube waveguide arrays on graphene films for local optical excitation on biological cells

NASA Astrophysics Data System (ADS)

Baek, Hyeonjun; Kwak, Hankyul; Song, Minho S.; Ha, Go Eun; Park, Jongwoo; Tchoe, Youngbin; Hyun, Jerome K.; Park, Hye Yoon; Cheong, Eunji; Yi, Gyu-Chul

2017-04-01

We report on scalable and position-controlled optical nanoprobe arrays using ZnO nanotube waveguides on graphene films for use in local optical excitation. For the waveguide fabrication, position-controlled and well-ordered ZnO nanotube arrays were grown on chemical vapor deposited graphene films with a submicron patterned mask layer and Au prepared between the interspace of nanotubes. Mammalian cells were cultured on the nanotube waveguide arrays and were locally excited by light illuminated through the nanotubes. Fluorescence and optogenetic signals could be excited through the optical nanoprobes. This method offers the ability to investigate cellular behavior with a high spatial resolution that surpasses the current limitation.

Investigation of the feasibility of temperature profiling optical diagnostics in the SSME fuel pre-burner

NASA Technical Reports Server (NTRS)

Shirley, J. A.

1983-01-01

Results of an analytical investigation to determine the feasibility of temperature profiling in the space shuttle main engine (SSME) fuel preburner are presented. In this application it is desirable to measure temperature in the preburner combustor with a remote, nonintrusive optical technique. Several techniques using laser excitation were examined with a consideration of the constraints imposed by optical access in the fuel preburner and the problems associated with operation near the functioning space shuttle engine. The potential performance of practical diagnostic systems based on spontaneous Raman backscattering, laser induced fluorescence, and coherent anti-Stokes Raman spectroscopy were compared analytically. A system using collection of spontaneous Raman backscattering excited by a remotely located 5 to 10 watt laser propagated to the SSME through a small diameter optical fiber was selected as the best approach. Difficulties normally associated with Raman scattering: weak signal strength and interference due to background radiation are not expected to be problematic due to the very high density in this application, and the low flame luminosity expected in the fuel rich hydrogen oxygen flame.

Quasiparticle Representation of Coherent Nonlinear Optical Signals of Multiexcitons

NASA Astrophysics Data System (ADS)

Fingerhut, Benjamin; Bennet, Kochise; Roslyak, Oleksiy; Mukamel, Shaul

2013-03-01

Elementary excitations of many-Fermion systems can be described within the quasiparticle approach which is widely used in the calculation of transport and optical properties of metals, semiconductors, molecular aggregates and strongly correlated quantum materials. The excitations are then viewed as independent harmonic oscillators where the many-body interactions between the oscillators are mapped into anharmonicities. We present a Green's function approach based on coboson algebra for calculating nonlinear optical signals and apply it onwards the study of two and three exciton states. The method only requires the diagonalization of the single exciton manifold and avoids equations of motion of multi-exciton manifolds. Using coboson algebra many body effects are recast in terms of tetradic exciton-exciton interactions: Coulomb scattering and Pauli exchange. The physical space of Fermions is recovered by singular-value decomposition of the over-complete coboson basis set. The approach is used to calculate third and fifth order quantum coherence optical signals that directly probe correlations in two- and three exciton states and their projections on the two and single exciton manifold.

Vibronic coupling in the excited-states of carotenoids

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

Miki, Takeshi; Buckup, Tiago; Krause, Marie S.

2016-01-01

The ultrafast femtochemistry of carotenoids is governed by the interaction between electronic excited states, which has been explained by the relaxation dynamics within a few hundred femtoseconds from the lowest optically allowed excited state S 2to the optically dark state S 1.

Vibronic coupling in the excited-states of carotenoids

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

Miki, Takeshi; Buckup, Tiago; Krause, Marie S.

The ultrafast femtochemistry of carotenoids is governed by the interaction between electronic excited states, which has been explained by the relaxation dynamics within a few hundred femtoseconds from the lowest optically allowed excited state S 2to the optically dark state S 1.

Coherent Excitation of Optical Phonons in GaAs by Broadband Terahertz Pulses

PubMed Central

Fu, Zhengping; Yamaguchi, Masashi

2016-01-01

Coherent excitation and control of lattice motion by electromagnetic radiation in optical frequency range has been reported through variety of indirect interaction mechanisms with phonon modes. However, coherent phonon excitation by direct interaction of electromagnetic radiation and nuclei has not been demonstrated experimentally in terahertz (THz) frequency range mainly due to the lack of THz emitters with broad bandwidth suitable for the purpose. We report the experimental observation of coherent phonon excitation and detection in GaAs using ultrafast THz-pump/optical-probe scheme. From the results of THz pump field dependence, pump/probe polarization dependence, and crystal orientation dependence, we attributed THz wave absorption and linear electro-optic effect to the excitation and detection mechanisms of coherent polar TO phonons. Furthermore, the carrier density dependence of the interaction of coherent phonons and free carriers is reported. PMID:27905563

Many-electron effects in the optical properties of single-walled carbon nanotubes

NASA Astrophysics Data System (ADS)

Spataru, Catalin D.; Ismail-Beigi, Sohrab; Capaz, Rodrigo B.; Louie, Steven G.

2005-03-01

Recent optical measurements on single-wall carbon nanotubes (SWCNT) showed anomalous behaviors that are indicative of strong many-electron effects. To understand these data, we performed ab initio calculation of self-energy and electron-hole interaction (excitonic) effects on the optical spectra of several SWCNTs. We employed a many-electron Green's function approach that determines both the quasiparticle and optical excitations from first principles. We found important many-electron effects that explain many of the puzzling experimental findings in the optical spectrum of these quasi-one dimensional systems, and are in excellent quantitative agreement with measurements. We have also calculated the radiative lifetime of the bright excitons in these tubes. Taking into account temperature effects and the existence of dark excitons, our results explain the radiative lifetime of excited nanotubes measured in time- resolved fluorescence experiments. This work was supported by the NSF under Grant No. DMR04-39768, and the U.S. DOE under Contract No. DE-AC03-76SF00098. Computational resources have been provided by NERSC and NPACI. RBC acknowledges financial support from the Guggenheim Foundation and Brazilian funding agencies CNPq, CAPES, FAPERJ, Instituto de Nanociências, FUJB-UFRJ and PRONEX-MCT.

Optical study of Erbium-doped-porous silicon based planar waveguides

NASA Astrophysics Data System (ADS)

Najar, A.; Ajlani, H.; Charrier, J.; Lorrain, N.; Haesaert, S.; Oueslati, M.; Haji, L.

2007-06-01

Planar waveguides were formed from porous silicon layers obtained on P + substrates. These waveguides were then doped by erbium using an electrochemical method. Erbium concentration in the range 2.2-2.5 at% was determined by energy dispersive X-ray (EDX) analysis performed on SEM cross sections. The refractive index of layers was studied before and after doping and thermal treatments. The photoluminescence of Er 3+ ions in the IR range and the decay curve of the 1.53 μm emission peak were studied as a function of the excitation power. The value of excited Er density was equal to 0.07%. Optical loss contributions were analyzed on these waveguides and the losses were equal to 1.1 dB/cm at 1.55 μm after doping.

Watching electrons tunnel

NASA Astrophysics Data System (ADS)

Moser, Simon

2008-03-01

To get insight to time resolved inner atomic or molecular processes, laser pulses of few femtoseconds or even attoseconds are needed. These short light pulse techniques ask for broad frequency spectra, control of dispersion and control of phase. Hence, linear optics fails and nonlinear optics in high electromagnetic fields is needed to satisfy the amount of control that is needed. One recent application of attosecond laser pulses is time resolved visualization of tunnel ionization in atoms applied to high electromagnetic fields. Here, Ne atom electrons are excited by an extreme ultraviolet attosecond laser pulse. After a while, a few cycles nearly infrared femtosecond laser pulse is applied to the atom causing tunnel ionization. The ion yield distribution can be measured as function of the delay time between excitation and ionization and so deliver insight to the time resolved mechanisms.

Building the analytical response in frequency domain of AC biased bolometers. Application to Planck/HFI

NASA Astrophysics Data System (ADS)

Sauvé, Alexandre; Montier, Ludovic

2016-12-01

Context: Bolometers are high sensitivity detector commonly used in Infrared astronomy. The HFI instrument of the Planck satellite makes extensive use of them, but after the satellite launch two electronic related problems revealed critical. First an unexpected excess response of detectors at low optical excitation frequency for ν < 1 Hz, and secondly the Analog To digital Converter (ADC) component had been insufficiently characterized on-ground. These two problems require an exquisite knowledge of detector response. However bolometers have highly nonlinear characteristics, coming from their electrical and thermal coupling making them very difficult to model. Goal: We present a method to build the analytical transfer function in frequency domain which describe the voltage response of an Alternative Current (AC) biased bolometer to optical excitation, based on the standard bolometer model. This model is built using the setup of the Planck/HFI instrument and offers the major improvement of being based on a physical model rather than the currently in use had-hoc model based on Direct Current (DC) bolometer theory. Method: The analytical transfer function expression will be presented in matrix form. For this purpose, we build linearized versions of the bolometer electro thermal equilibrium. A custom description of signals in frequency is used to solve the problem with linear algebra. The model performances is validated using time domain simulations. Results: The provided expression is suitable for calibration and data processing. It can also be used to provide constraints for fitting optical transfer function using real data from steady state electronic response and optical response. The accurate description of electronic response can also be used to improve the ADC nonlinearity correction for quickly varying optical signals.

Dark solitons in the condensate of exciton polaritons in semiconductor microcavities under nonresonant optical excitation

NASA Astrophysics Data System (ADS)

Demenev, A. A.; Gavrilov, S. S.; Brichkin, A. S.; Larionov, A. V.; Kulakovskii, V. D.

2014-12-01

The first-order spatial correlation function g (1)( r 12) and the polariton density distribution in the condensate of quasi-two-dimensional exciton polaritons formed in a high- Q semiconductor microcavity pillar under nonresonant optical pumping are investigated. It is found that the correlation function in certain regions of the micropillar decreases abruptly with increasing condensate density. It is shown that this behavior of the correlation function is caused by the formation of a localized dark soliton in these regions. A deep minimum of the polariton density and a shift in the phase of the condensate wavefunction by π occur within the soliton localization area.

Analysis of Cervical Supernatant Samples Luminescence Using 355 nm Laser

NASA Astrophysics Data System (ADS)

Vaitkuviene, A.; Gegzna, V.; Kurtinaitiene, R.; Stanikunas, R.; Rimiene, J.; Vaitkus, J.

2010-05-01

The biomarker discovery for accurate detection and diagnosis of cervical carcinoma and its malignant precursors represents one of the current challenges in clinical medicine. Laser induced autofluorescence spectra in cervical smear content were fitted to predict the cervical epithelium diagnosis as a lab off "optical biopsy" method. Liquid PAP supernatant sediment dried on Quartz plate spectroscopy was performed by 355 nm Nd YAG microlaser STA-1 (Standa, Ltd). For comparison a liquid supernatant spectroscopy was formed by laboratory "Perkin Elmer LS 50B spetrometer at 290, 300, 310 nm excitations. Analysis of spectrum was performed by approximation using the multi-peaks program with Lorentz functions for the liquid samples and with Gaussian functions for the dry samples. Ratio of spectral components area to the area under whole experimental curve (SPP) was calculated. The spectral components were compared by averages of SPP using Mann-Whitney U-test in histology groups. Results. Differentiation of Normal and HSIL/CIN2+ cases in whole supernatant could be performed by stationary laboratory lamp spectroscopy at excitation 290 nm and emission >379 nm with accuracy AUC 0,69, Sens 0,72, Spec 0,65. Differentiation Normal versus HSIL/CIN2+ groups in dried enriched supernatant could be performed by 355 nm microlaser excitation at emission 405-424 nm with accuracy (AUC 0,96, Sens 0,91, Spec 1.00). Diagnostic algorithm could be created for all histology groups differentiation under 355 nm excitation. Microlaser induced "optical biopsy "looks promising method for cervical screening at the point of care.

Generation of terahertz from ZnGeP2 crystal and its application to record the time-resolved photoacoustic spectra of nitromethane

NASA Astrophysics Data System (ADS)

Rao, K. S.; Ganesh, D.; Chaudhary, A. K.

2018-07-01

This paper reports the generation of THz radiation through the optical rectification process from type-I cut Zinc germanium phosphate (ZnGeP2or ZGP) crystal using optical parametric amplifier pulses (tunable between 1.15-1.6 μm range, at 60 fs pulse duration and 1 kHz repetition rate) as pump wavelengths at an average power of 50 mW. Also, we have ascertained the conversion efficiency of the generated THz signal, which is of the order of 0.62% at 1.5 THz. Further, the generated radiation is employed for the recording of absorption bands (in terms of PA spectra) of nitromethane and methanol vapor at room temperature using bandpass filters having central frequencies of 0.5 and 1.5 THz. In addition, we have employed the UV-266 nm as an excitation wavelength to record the time domain photoacoustic (PA) spectra of nitromethane (CH3NO2). In case of UV and THz radiations, the excitation mechanisms follow strong electronic (π∗ ← n) and weak vibrational-rotational due to ultrafast transition, respectively. In case of UV-266 nm the characteristic PA spectra has been also presented as a function of vapor pressure and data acquisition time with two different PA cells. The current study reveals the effect of the nanoseconds and the ultrafast pulses on some of the common excited acoustic modes (due to similar functional group), which follow two different types of excitation mechanism.

Optical Absorption in Molecular Crystals from Time-Dependent Density Functional Theory

DTIC Science & Technology

2017-04-18

fundamental gap but there is little effect on the optical spectra. We therefore believe that the method is robust and can be used for studies of... quantitative DFT- based prediction of excited-state properties in molecu- lar solids.[28, 29] In this approach, one first computes the underlying gas...gradient ap- proximation (GGA). In some cases , the fraction of SR Fock exchange, α, can be determined from first-principles based on satisfaction of

PDT dose dosimetry for Photofrin-mediated pleural photodynamic therapy (pPDT)

NASA Astrophysics Data System (ADS)

Ong, Yi Hong; Kim, Michele M.; Finlay, Jarod C.; Dimofte, Andreea; Singhal, Sunil; Glatstein, Eli; Cengel, Keith A.; Zhu, Timothy C.

2018-01-01

Photosensitizer fluorescence excited by photodynamic therapy (PDT) treatment light can be used to monitor the in vivo concentration of the photosensitizer and its photobleaching. The temporal integral of the product of in vivo photosensitizer concentration and light fluence is called PDT dose, which is an important dosimetry quantity for PDT. However, the detected photosensitizer fluorescence may be distorted by variations in the absorption and scattering of both excitation and fluorescence light in tissue. Therefore, correction of the measured fluorescence for distortion due to variable optical properties is required for absolute quantification of photosensitizer concentration. In this study, we have developed a four-channel PDT dose dosimetry system to simultaneously acquire light dosimetry and photosensitizer fluorescence data. We measured PDT dose at four sites in the pleural cavity during pleural PDT. We have determined an empirical optical property correction function using Monte Carlo simulations of fluorescence for a range of physiologically relevant tissue optical properties. Parameters of the optical property correction function for Photofrin fluorescence were determined experimentally using tissue-simulating phantoms. In vivo measurements of photosensitizer fluorescence showed negligible photobleaching of Photofrin during the PDT treatment, but large intra- and inter-patient heterogeneities of in vivo Photofrin concentration are observed. PDT doses delivered to 22 sites in the pleural cavity of 8 patients were different by 2.9 times intra-patient and 8.3 times inter-patient.

Two-color CW STED nanoscopy

NASA Astrophysics Data System (ADS)

Chen, Xuanze; Liu, Yujia; Yang, Xusan; Wang, Tingting; Alonas, Eric; Santangelo, Philip J.; Ren, Qiushi; Xi, Peng

2013-02-01

Fluorescent microscopy has become an essential tool to study biological molecules, pathways and events in living cells, tissues and animals. Meanwhile even the most advanced confocal microscopy can only yield optical resolution approaching Abbe diffraction limit of 200 nm. This is still larger than many subcellular structures, which are too small to be resolved in detail. These limitations have driven the development of super-resolution optical imaging methodologies over the past decade. In stimulated emission depletion (STED) microscopy, the excitation focus is overlapped by an intense doughnut-shaped spot to instantly de-excite markers from their fluorescent state to the ground state by stimulated emission. This effectively eliminates the periphery of the Point Spread Function (PSF), resulting in a narrower focal region, or super-resolution. Scanning a sharpened spot through the specimen renders images with sub-diffraction resolution. Multi-color STED imaging can present important structural and functional information for protein-protein interaction. In this work, we presented a two-color, synchronization-free STED microscopy with a Ti:Sapphire oscillator. The excitation wavelengths were 532nm and 635nm, respectively. With pump power of 4.6 W and sample irradiance of 310 mW, we achieved super-resolution as high as 71 nm. Human respiratory syncytial virus (hRSV) proteins were imaged with our two-color CW STED for co-localization analysis.

Electronic and optical properties of hexathiapentacene in the gas and crystal phases

NASA Astrophysics Data System (ADS)

Cardia, R.; Malloci, G.; Rignanese, G.-M.; Blase, X.; Molteni, E.; Cappellini, G.

2016-06-01

Using density functional theory (DFT) and its time-dependent (TD) extension, the electronic and optical properties of the hexathiapentacene (HTP) molecule, a derivative of pentacene (PNT) obtained by symmetric substitution of the six central H atoms with S atoms, are investigated for its gas and solid phases. For the molecular structure, all-electron calculations are performed using a Gaussian localized orbital basis set in conjunction with the Becke three-parameter Lee-Yang-Parr (B3LYP) hybrid exchange-correlation functional. Electron affinities, ionization energies, quasiparticle energy gaps, optical absorption spectra, and exciton binding energies are calculated and compared with the corresponding results for PNT, as well as with the available experimental data. The DFT and TDDFT results are also validated by performing many-body perturbation theory calculations within the G W and Bethe-Salpeter equation formalisms. The functionalization with S atoms induces an increase of both ionization energies and electron affinities, a sizable reduction of the fundamental electronic gap, and a redshift of the optical absorption onset. Notably, the intensity of the first absorption peak of HTP falling in the visible region is found to be nearly tripled with respect to the pure PNT molecule. For the crystal structures, pseudopotential calculations are adopted using a plane-wave basis set together with the Perdew-Burke-Ernzerhof exchange-correlation functional empirically corrected in order to take dispersive interactions into account. The electronic excitations are also obtained within a perturbative B3LYP scheme. A comparative analysis is carried out between the ground-state and excited-state properties of crystalline HTP and PNT linking to the findings obtained for the isolated molecules.

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.

Optical filters for wavelength selection in fluorescence instrumentation.

PubMed

Erdogan, Turan

2011-04-01

Fluorescence imaging and analysis techniques have become ubiquitous in life science research, and they are poised to play an equally vital role in in vitro diagnostics (IVD) in the future. Optical filters are crucial for nearly all fluorescence microscopes and instruments, not only to provide the obvious function of spectral control, but also to ensure the highest possible detection sensitivity and imaging resolution. Filters make it possible for the sample to "see" light within only the absorption band, and the detector to "see" light within only the emission band. Without filters, the detector would not be able to distinguish the desired fluorescence from scattered excitation light and autofluorescence from the sample, substrate, and other optics in the system. Today the vast majority of fluorescence instruments, including the widely popular fluorescence microscope, use thin-film interference filters to control the spectra of the excitation and emission light. Hence, this unit emphasizes thin-film filters. After briefly introducing different types of thin-film filters and how they are made, the unit describes in detail different optical filter configurations in fluorescence instruments, including both single-color and multicolor imaging systems. Several key properties of thin-film filters, which can significantly affect optical system performance, are then described. In the final section, tunable optical filters are also addressed in a relative comparison.

Imaging of Brain Slices with a Genetically Encoded Voltage Indicator.

PubMed

Quicke, Peter; Barnes, Samuel J; Knöpfel, Thomas

2017-01-01

Functional fluorescence microscopy of brain slices using voltage sensitive fluorescent proteins (VSFPs) allows large scale electrophysiological monitoring of neuronal excitation and inhibition. We describe the equipment and techniques needed to successfully record functional responses optical voltage signals from cells expressing a voltage indicator such as VSFP Butterfly 1.2. We also discuss the advantages of voltage imaging and the challenges it presents.

Predictive assessment of kidney functional recovery following ischemic injury using optical spectroscopy

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

Raman, Rajesh N.; Pivetti, Christopher D.; Ramsamooj, Rajendra

Functional changes in rat kidneys during the induced ischemic injury and recovery phases were explored using multimodal autofluorescence and light scattering imaging. We aim to evaluate the use of noncontact optical signatures for rapid assessment of tissue function and viability. Specifically, autofluorescence images were acquired in vivo under 355, 325, and 266 nm illumination while light scattering images were collected at the excitation wavelengths as well as using relatively narrowband light centered at 500 nm. The images were simultaneously recorded using a multimodal optical imaging system. We also analyzed to obtain time constants, which were correlated to kidney dysfunction asmore » determined by a subsequent survival study and histopathological analysis. This analysis of both the light scattering and autofluorescence images suggests that changes in tissue microstructure, fluorophore emission, and blood absorption spectral characteristics, coupled with vascular response, contribute to the behavior of the observed signal, which may be used to obtain tissue functional information and offer the ability to predict posttransplant kidney function.« less

Predictive assessment of kidney functional recovery following ischemic injury using optical spectroscopy

DOE PAGES

Raman, Rajesh N.; Pivetti, Christopher D.; Ramsamooj, Rajendra; ...

2017-05-03

Functional changes in rat kidneys during the induced ischemic injury and recovery phases were explored using multimodal autofluorescence and light scattering imaging. We aim to evaluate the use of noncontact optical signatures for rapid assessment of tissue function and viability. Specifically, autofluorescence images were acquired in vivo under 355, 325, and 266 nm illumination while light scattering images were collected at the excitation wavelengths as well as using relatively narrowband light centered at 500 nm. The images were simultaneously recorded using a multimodal optical imaging system. We also analyzed to obtain time constants, which were correlated to kidney dysfunction asmore » determined by a subsequent survival study and histopathological analysis. This analysis of both the light scattering and autofluorescence images suggests that changes in tissue microstructure, fluorophore emission, and blood absorption spectral characteristics, coupled with vascular response, contribute to the behavior of the observed signal, which may be used to obtain tissue functional information and offer the ability to predict posttransplant kidney function.« less

Multimodal instrument for high-sensitivity autofluorescence and spectral optical coherence tomography of the human eye fundus

PubMed Central

Komar, Katarzyna; Stremplewski, Patrycjusz; Motoczyńska, Marta; Szkulmowski, Maciej; Wojtkowski, Maciej

2013-01-01

In this paper we present a multimodal device for imaging fundus of human eye in vivo which combines functionality of autofluorescence by confocal SLO with Fourier domain OCT. Native fluorescence of human fundus was excited by modulated laser beam (λ = 473 nm, 20 MHz) and lock-in detection was applied resulting in improving sensitivity. The setup allows for acquisition of high resolution OCT and high contrast AF images using fluorescence excitation power of 50-65 μW without averaging consecutive images. Successful functioning of constructed device have been demonstrated for 8 healthy volunteers of different age ranging from 24 to 83 years old. PMID:24298426

Eyecup scope—optical recordings of light stimulus-evoked fluorescence signals in the retina

PubMed Central

Hausselt, Susanne E.; Breuninger, Tobias; Castell, Xavier; Denk, Winfried; Margolis, David J.; Detwiler, Peter B.

2009-01-01

Dendritic signals play an essential role in processing visual information in the retina. To study them in neurites too small for electrical recording, we developed an instrument that combines a multi-photon (MP) microscope with a through-the-objective high-resolution visual stimulator. An upright microscope was designed that uses the objective lens for both MP imaging and delivery of visual stimuli to functionally intact retinal explants or eyecup preparations. The stimulator consists of a miniature liquid-crystal-on-silicon display coupled into the optical path of an infrared-excitation laser-scanning microscope. A pair of custom-made dichroic filters allows light from the excitation laser and three spectral bands (‘colors’) from the stimulator to reach the retina, leaving two intermediate bands for fluorescence imaging. Special optics allow displacement of the stimulator focus relative to the imaging focus. Spatially resolved changes in calcium-indicator fluorescence in response to visual stimuli were recorded in dendrites of different types of mammalian retinal neurons. PMID:19023590

Defect states in hexagonal boron nitride: Assignments of observed properties and prediction of properties relevant to quantum computation

NASA Astrophysics Data System (ADS)

Sajid, A.; Reimers, Jeffrey R.; Ford, Michael J.

2018-02-01

Key properties of nine possible defect sites in hexagonal boron nitride (h-BN), VN,VN -1,CN,VNO2 B,VNNB,VNCB,VBCN,VBCNS iN , and VNCBS iB , are predicted using density-functional theory and are corrected by applying results from high-level ab initio calculations. Observed h-BN electron-paramagnetic resonance signals at 22.4, 20.83, and 352.70 MHz are assigned to VN,CN, and VNO2 B , respectively, while the observed photoemission at 1.95 eV is assigned to VNCB . Detailed consideration of the available excited states, allowed spin-orbit couplings, zero-field splitting, and optical transitions is made for the two related defects VNCB and VBCN . VNCB is proposed for realizing long-lived quantum memory in h-BN. VBCN is predicted to have a triplet ground state, implying that spin initialization by optical means is feasible and suitable optical excitations are identified, making this defect of interest for possible quantum-qubit operations.

Charge transport in organic multi-layer devices under electric and optical fields

NASA Astrophysics Data System (ADS)

Park, June Hyoung

2007-12-01

Charge transport in small organic molecules and conjugated conducting polymers under electric or optical fields is studied by using field effect transistors and photo-voltaic cells with multiple thin layers. With these devices, current under electric field, photo-current under optical field, and luminescence of optical materials are measured to characterize organic and polymeric materials. For electric transport studies, poly(3,4-ethylenedioxythiophene) doped by polystyrenesulfonic acid is used, which is conductive with conductivity of approximately 25 S/cm. Despite their high conductance, field effect transistors based on the films are successfully built and characterized by monitoring modulations of drain current by gate voltage and IV characteristic curves. Due to very thin insulating layers of poly(vinylphenol), the transistors are relative fast under small gate voltage variation although heavy ions are involved in charge transport. In IV characteristic curves, saturation effects can be observed. Analysis using conventional field effect transistor model indicates high mobility of charge carriers, 10 cm2/V·sec, which is not consistent with the mobility of the conducting polymer. It is proposed that the effect of a small density of ions injected via polymer dielectric upon application of gate voltage and the ion compensation of key hopping sites accounts for the operation of the field effect transistors. For the studies of transport under optical field, photovoltaic cells with 3 different dendrons, which are efficient to harvest photo-excited electrons, are used. These dendrons consist of two electron-donors (tetraphenylporphyrin) and one electron-accepter (naphthalenediimide). Steady-state fluorescence measurements show that inter-molecular interaction is dominant in solid dendron film, although intra-molecular interaction is still present. Intra-molecular interaction is suggested by different fluorescence lifetimes between solutions of donor and dendrons. This intra-molecular interaction has two processes, transport via pi-stackings and transport via linking functional groups in the dendrons. IV characteristic spectra of the photovoltaic cells suggest that the transport route of photo-excited charges depends on wavelength of incident light on the cells. For excitation by the Soret band and the lowest Q band, a photo-excited electron can transport directly to a neighbor dendron. For excitation by high-energy Q bands, a photo-excited electron transports via the electron-accepters.

Spectroscopy of the three-photon laser excitation of cold Rubidium Rydberg atoms in a magneto-optical trap

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

Entin, V. M.; Yakshina, E. A.; Tretyakov, D. B.

2013-05-15

The spectra of the three-photon laser excitation 5S{sub 1/2} {yields} 5P{sub 3/2} {yields} 6S{sub 1/2}nP of cold Rb Rydberg atoms in an operating magneto-optical trap based on continuous single-frequency lasers at each stage are studied. These spectra contain two partly overlapping peaks of different amplitudes, which correspond to coherent three-photon excitation and incoherent three-step excitation due to the presence of two different ways of excitation through the dressed states of intermediate levels. A four-level theoretical model based on optical Bloch equations is developed to analyze these spectra. Good agreement between the experimental and calculated data is achieved by introducing additionalmore » decay of optical coherence induced by a finite laser line width and other broadening sources (stray electromagnetic fields, residual Doppler broadening, interatomic interactions) into the model.« less

Effect of different surfactants on structural and optical properties of Ce3+ and Tb3+ co-doped BiPO4 nanostructures

NASA Astrophysics Data System (ADS)

Lakshminarayana, G.; Dao, T. D.; Chen, K.; Sharma, Manoj; Takeda, T.; Brik, M. G.; Kityk, I. V.; Singh, Sarabjot; Nagao, T.

2015-01-01

In this paper we report on the Ce3+ and Tb3+ ions co-doped bismuth phosphate (BiPO4) nanostructures that were synthesized by a simple precipitation method using different surfactants such as glycerol/H2O, glycerol/ethylene glycol, oleic acid, and ethylene glycol. The structural (X-ray diffraction, scanning electron microscopy, tunneling electron microscopy), functional groups analysis (Fourier transform infrared and Raman spectroscopy), thermal (thermogravimetry and differential thermal analysis), and optical (photoluminescence, photoluminescence-excitation) properties were investigated. The structural and morphological analysis confirms the pure hexagonal crystal structure of the synthesized nanostructures. From the measured Fourier transform infrared (FTIR) and Raman spectra various functional groups such as υ3 stretching vibration of the PO4 group, and δ(O-P-O) and υ4 (PO4) vibrations including the υ2 and υ1 bending modes of the PO4 units are identified. Based on the thermal analysis, for all the studied samples an exothermic peak between 680 °C and 700 °C was observed due to phase transition from hexagonal to high temperature monoclinic. The Ce3+and Tb3+ codoped samples show spectrally broad 5d → 4f luminescence in the blue (centered at 459 nm) wavelength region under the direct optical excitation of Ce3+ at 417 nm. Similarly, Tb3+ has revealed four main emission bands (5D4 → 7F6, 5, 4 and 3) at 490 nm, 545 nm, 585 nm and 621 nm with 378 nm (7F6 → 5G6) as the excitation wavelength, including three more weak emission bands at 647 nm, 669 nm, and 681 nm which could be assigned to 5D4 → 7F2, 1, 0 emission transitions. Among them, 545 nm (5D4 → 7F5) has shown bright green emission. The Ce3+ and Tb3+ codoped sample synthesized with pure oleic acid have shown relatively high green emission intensity for Tb3+, and relatively weak blue emission intensity for Ce3+ under their respective optical excitation wavelengths.

Optical fingerprint of non-covalently functionalized transition metal dichalcogenides

NASA Astrophysics Data System (ADS)

Feierabend, Maja; Malic, Ermin; Knorr, Andreas; Berghäuser, Gunnar

2017-09-01

Atomically thin transition metal dichalcogenides (TMDs) hold promising potential for applications in optoelectronics. Due to their direct band gap and the extraordinarily strong Coulomb interaction, TMDs exhibit efficient light-matter coupling and tightly bound excitons. Moreover, large spin orbit coupling in combination with circular dichroism allows for spin and valley selective optical excitation. As atomically thin materials, they are very sensitive to changes in the surrounding environment. This motivates a functionalization approach, where external molecules are adsorbed to the materials surface to tailor its optical properties. Here, we apply the density matrix theory to investigate the potential of non-covalently functionalized monolayer TMDs. Considering exemplary molecules with a strong dipole moment, we predict spectral redshifts and the appearance of an additional side peak in the absorption spectrum of functionalized TMDs. We show that the molecular characteristics, e.g. coverage, orientation and dipole moment, crucially influence the optical properties of TMDs, leaving a unique optical fingerprint in the absorption spectrum. Furthermore, we find that the molecular dipole moments open a channel for coherent intervalley coupling between the high-symmetry K and K\\prime points which may create new possibilities for spin-valleytronics application.

Optical nonlinearities in plasmonic metamaterials (Conference Presentation)

NASA Astrophysics Data System (ADS)

Zayats, Anatoly V.

2016-04-01

Metals exhibit strong and fast nonlinearities making metallic, plasmonic, structures very promising for ultrafast all-optical applications at low light intensities. Combining metallic nanostructures in metamaterials provides additional functionalities via prospect of precise engineering of spectral response and dispersion. From this point of view, hyperbolic metamaterials, in particular those based on plasmonic nanorod arrays, provide wealth of exciting possibilities in nonlinear optics offering designed linear and nonlinear properties, polarization control, spontaneous emission control and many others. Experiments and modeling have already demonstrated very strong Kerr-nonlinear response and its ultrafast recovery due to the nonlocal nature of the plasmonic mode of the metamaterial, so that small changes in the permittivity of the metallic component under the excitation modify the nonlocal response that in turn leads to strong changes of the metamaterial transmission. In this talk, we will discuss experimental studies and numerical modeling of second- and third-order nonlinear optical processes in hyperbolic metamaterials based on metallic nanorods and other plasmonic systems where coupling between the resonances plays important role in defining nonlinear response. Second-harmonic generation and ultrafast Kerr-type nonlinearity originating from metallic component of the metamaterial will be considered, including nonlinear magneto-optical effects. Nonlinear optical response of stand-alone as well as integrated metamaterial components will be presented. Some of the examples to be discussed include nonlinear polarization control, nonlinear metamaterial integrated in silicon photonic circuitry and second-harmonic generation, including magneto-optical effects.

A hybrid electromagnetic-acoustic levitator for the containerless processing of undercooled melts

NASA Technical Reports Server (NTRS)

Hmelo, Anthony B.; Banerjee, Sharbari; Wang, Taylor G.

1992-01-01

The hybrid, acoustic-EM levitator discussed provides a small lifting force independently of its EM component by exciting an acoustic resonance that serves as a pressure node at the position of the EM-levitated specimen. The system also stabilizes and damps chaotic oscillations during specimen positioning, and can excite forced oscillations of levitated molten metals for drop-physics and thermophysical property measurements. Attention is given to the character and function of the atmosphere in the levitator. Noncontact temperature measurement is via single-color optical pyrometer.

Dual modality instrument for simultaneous optical coherence tomography imaging and fluorescence spectroscopy.

PubMed

Barton, Jennifer Kehlet; Guzman, Francisco; Tumlinson, Alexandre

2004-01-01

We develop a dual-modality device that combines the anatomical imaging capabilities of optical coherence tomography (OCT) with the functional capabilities of laser-induced fluorescence (LIF) spectroscopy. OCT provides cross-sectional images of tissue structure to a depth of up to 2 mm with approximately 10-microm resolution. LIF spectroscopy provides histochemical information in the form of emission spectra from a given tissue location. The OCT subsystem utilizes a superluminescent diode with a center wavelength of 1300 nm, whereas a helium cadmium laser provides the LIF excitation source at wavelengths of 325 and 442 nm. Preliminary data are obtained on eight postmortem aorta samples, each 10 mm in length. OCT images and LIF spectra give complementary information from normal and atherosclerotic portions of aorta wall. OCT images show structures such as intima, media, internal elastic lamina, and fibrotic regions. Emission spectra ratios of 520/490 (325-nm excitation) and 595/635 (442-nm excitation) could be used to identify normal and plaque regions with 97 and 91% correct classification rates, respectively. With miniaturization of the delivery probe and improvements in system speed, this dual-modality device could provide a valuable tool for identification and characterization of atherosclerotic plaques. (c) 2004 Society of Photo-Optical Instrumentation Engineers.

X-ray Excitation Triggers Ytterbium Anomalous Emission in CaF2:Yb but Not in SrF2:Yb.

PubMed

Hughes-Currie, Rosa B; Ivanovskikh, Konstantin V; Wells, Jon-Paul R; Reid, Michael F; Gordon, Robert A; Seijo, Luis; Barandiarán, Zoila

2017-03-16

Materials that luminesce after excitation with ionizing radiation are extensively applied in physics, medicine, security, and industry. Lanthanide dopants are known to trigger crystal scintillation through their fast d-f emissions; the same is true for other important applications as lasers or phosphors for lighting. However, this ability can be seriously compromised by unwanted anomalous emissions often found with the most common lanthanide activators. We report high-resolution X-ray-excited optical (IR to UV) luminescence spectra of CaF 2 :Yb and SrF 2 :Yb samples excited at 8949 eV and 80 K. Ionizing radiation excites the known anomalous emission of ytterbium in the CaF 2 host but not in the SrF 2 host. Wave function-based ab initio calculations of host-to-dopant electron transfer and Yb 2+ /Yb 3+ intervalence charge transfer explain the difference. The model also explains the lack of anomalous emission in Yb-doped SrF 2 excited by VUV radiation.

Dynamic evolution of light-induced orientation of dye-doped liquid crystals in liquid phase studied by time-resolved optically heterodyned optical Kerr effect technique.

PubMed

Yang, Pei; Liu, Liying; Xu, Lei

2008-02-28

Transient evolution of light-induced molecular reorientation both in 1-amino-anthraquinone (1AAQ) dye and azobenzene doped isotropic liquid crystals (LCs) were studied by time-resolved optically heterodyned optical Kerr effect method. The results give clear direct experimental proof that under short pulse (30 ps) excitation, LC molecules orientate toward the excitation light polarization direction in the 1AAQ/LC system. However, LC molecular orientation becomes orthogonal to the light polarization in azobenzene/LC system. Time-resolved excited-state absorption of 1AAQ and wavelength dependent excited-state absorption of azobenzene were also observed and their contributions to the early dynamics of the third order optical responses of the two systems were confirmed. A simplified two-level mean-field theory was derived to reveal the intensity dependence of orientation enhancement factor in azobenzene/LC system considering the photoisomerization process.

Landau damping of Bogoliubov excitations in two- and three-dimensional optical lattices at finite temperatures

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

Tsuchiya, Shunji; Department of Physics, Waseda University, 3-4-1 Okubo, Tokyo 169-8555; Griffin, Allan

2005-11-15

We study the Landau damping of Bogoliubov excitations in two- and three-dimensional optical lattices at finite temperatures, extending our recent work on one-dimensional (1D) optical lattices. We use a Bose-Hubbard tight-binding model and the Popov approximation to calculate the temperature dependence of the number of condensate atoms n{sup c0}(T) in each lattice well. As with 1D optical lattices, damping only occurs if the Bogoliubov excitations exhibit anomalous dispersion (i.e., the excitation energy bends upward at low momentum), analogous to the case of phonons in superfluid {sup 4}He. This leads to the disappearance of all damping processes in a D-dimensional simplemore » cubic optical lattice when Un{sup c0}{>=}6DJ, where U is the on-site interaction, and J is the hopping matrix element.« less

Monte Carlo Simulations of Electron Energy-Loss Spectra with the Addition of Fine Structure from Density Functional Theory Calculations.

PubMed

Attarian Shandiz, Mohammad; Guinel, Maxime J-F; Ahmadi, Majid; Gauvin, Raynald

2016-02-01

A new approach is presented to introduce the fine structure of core-loss excitations into the electron energy-loss spectra of ionization edges by Monte Carlo simulations based on an optical oscillator model. The optical oscillator strength is refined using the calculated electron energy-loss near-edge structure by density functional theory calculations. This approach can predict the effects of multiple scattering and thickness on the fine structure of ionization edges. In addition, effects of the fitting range for background removal and the integration range under the ionization edge on signal-to-noise ratio are investigated.

Fiber optic biofluorometer for physiological research on muscle slices

NASA Astrophysics Data System (ADS)

Belz, Mathias; Dendorfer, Andreas; Werner, Jan; Lambertz, Daniel; Klein, Karl-Friedrich

2016-03-01

A focus of research in cell physiology is the detection of Ca2+, NADH, FAD, ATPase activity or membrane potential, only to name a few, in muscle tissues. In this work, we report on a biofluorometer using ultraviolet light emitting diodes (UV-LEDs), optical fibers and two photomultipliers (PMTs) using synchronized fluorescence detection with integrated background correction to detect free calcium, Ca2+, in cardiac muscle tissue placed in a horizontal tissue bath and a microscope setup. Fiber optic probes with imaging optics have been designed to transport excitation light from the biofluorometer's light output to a horizontal tissue bath and to collect emission light from a tissue sample of interest to two PMTs allowing either single excitation / single emission or ratiometric, dual excitation / single emission or single excitation / dual emission fluorescence detection of indicator dyes or natural fluorophores. The efficient transport of light from the excitation LEDs to the tissue sample, bleaching effects of the excitation light in both, polymer and fused silica-based fibers will be discussed. Furthermore, a new approach to maximize light collection of the emission light using high NA fibers and high NA coupling optics will be shown. Finally, first results on Ca2+ measurements in cardiac muscle slices in a traditional microscope setup and a horizontal tissue bath using fiber optic probes will be introduced and discussed.

A set of optical methods for studying marine phytoplankton

NASA Astrophysics Data System (ADS)

Konyukhov, I. V.; Glukhovets, D. I.

2017-05-01

The results of integrated optical measurements of Black Sea water samples using a spectrophotometer, laser spectrometer, and fluorometer with pulse-modulated excitation light are discussed. A linear correlation between the intensities of chlorophyll absorption at 673 nm and chlorophyll fluorescence (680-750 nm) is observed. Phycoerythrin-containing organisms are recorded in phytoplankton in layers below 20 m. The data of 1-week monitoring of phytoplankton abundance and functional activity in Golubaya Bay with a Mega-25 flow fluorometer are described.

Nano-optical conveyor belt with waveguide-coupled excitation.

PubMed

Wang, Guanghui; Ying, Zhoufeng; Ho, Ho-pui; Huang, Ying; Zou, Ningmu; Zhang, Xuping

2016-02-01

We propose a plasmonic nano-optical conveyor belt for peristaltic transport of nano-particles. Instead of illumination from the top, waveguide-coupled excitation is used for trapping particles with a higher degree of precision and flexibility. Graded nano-rods with individual dimensions coded to have resonance at specific wavelengths are incorporated along the waveguide in order to produce spatially addressable hot spots. Consequently, by switching the excitation wavelength sequentially, particles can be transported to adjacent optical traps along the waveguide. The feasibility of this design is analyzed using three-dimensional finite-difference time-domain and Maxwell stress tensor methods. Simulation results show that this system is capable of exciting addressable traps and moving particles in a peristaltic fashion with tens of nanometers resolution. It is the first, to the best of our knowledge, report about a nano-optical conveyor belt with waveguide-coupled excitation, which is very important for scalability and on-chip integration. The proposed approach offers a new design direction for integrated waveguide-based optical manipulation devices and its application in large scale lab-on-a-chip integration.

Plasmonic graded nano-disks as nano-optical conveyor belt.

PubMed

Kang, Zhiwen; Lu, Haifei; Chen, Jiajie; Chen, Kun; Xu, Fang; Ho, Ho-Pui

2014-08-11

We propose a plasmonic system consisting of nano-disks (NDs) with graded diameters for the realization of nano-optical conveyor belt. The system contains a couple of NDs with individual elements coded with different resonant wavelengths. By sequentially switching the wavelength and polarization of the excitation source, optically trapped target nano-particle can be transferred from one ND to another. The feasibility of such function is verified based on the three-dimensional finite-difference time-domain technique and the Maxwell stress tensor method. Our design may provide an alternative way to construct nano-optical conveyor belt with which target molecules can be delivered between trapping sites, thus enabling many on-chip optofluidic applications.

Three-Photon Luminescence of Gold Nanorods and Its Applications for High Contrast Tissue and Deep In Vivo Brain Imaging

PubMed Central

Wang, Shaowei; Xi, Wang; Cai, Fuhong; Zhao, Xinyuan; Xu, Zhengping; Qian, Jun; He, Sailing

2015-01-01

Gold nanoparticles can be used as contrast agents for bio-imaging applications. Here we studied multi-photon luminescence (MPL) of gold nanorods (GNRs), under the excitation of femtosecond (fs) lasers. GNRs functionalized with polyethylene glycol (PEG) molecules have high chemical and optical stability, and can be used as multi-photon luminescent nanoprobes for deep in vivo imaging of live animals. We have found that the depth of in vivo imaging is dependent upon the transmission and focal capability of the excitation light interacting with the GNRs. Our study focused on the comparison of MPL from GNRs with two different aspect ratios, as well as their ex vivo and in vivo imaging effects under 760 nm and 1000 nm excitation, respectively. Both of these wavelengths were located at an optically transparent window of biological tissue (700-1000 nm). PEGylated GNRs, which were intravenously injected into mice via the tail vein and accumulated in major organs and tumor tissue, showed high image contrast due to distinct three-photon luminescence (3PL) signals upon irradiation of a 1000 nm fs laser. Concerning in vivo mouse brain imaging, the 3PL imaging depth of GNRs under 1000 nm fs excitation could reach 600 μm, which was approximately 170 μm deeper than the two-photon luminescence (2PL) imaging depth of GNRs with a fs excitation of 760 nm. PMID:25553113

Cooperative photoinduced metastable phase control in strained manganite films

NASA Astrophysics Data System (ADS)

Zhang, Jingdi; Tan, Xuelian; Liu, Mengkun; Teitelbaum, S. W.; Post, K. W.; Jin, Feng; Nelson, K. A.; Basov, D. N.; Wu, Wenbin; Averitt, R. D.

2016-09-01

A major challenge in condensed-matter physics is active control of quantum phases. Dynamic control with pulsed electromagnetic fields can overcome energetic barriers, enabling access to transient or metastable states that are not thermally accessible. Here we demonstrate strain-engineered tuning of La2/3Ca1/3MnO3 into an emergent charge-ordered insulating phase with extreme photo-susceptibility, where even a single optical pulse can initiate a transition to a long-lived metastable hidden metallic phase. Comprehensive single-shot pulsed excitation measurements demonstrate that the transition is cooperative and ultrafast, requiring a critical absorbed photon density to activate local charge excitations that mediate magnetic-lattice coupling that, in turn, stabilize the metallic phase. These results reveal that strain engineering can tune emergent functionality towards proximal macroscopic states to enable dynamic ultrafast optical phase switching and control.

Fiber pigtailed thin wall capillary coupler for excitation of microsphere WGM resonator.

PubMed

Wang, Hanzheng; Lan, Xinwei; Huang, Jie; Yuan, Lei; Kim, Cheol-Woon; Xiao, Hai

2013-07-01

In this paper, we demonstrate a fiber pigtailed thin wall capillary coupler for excitation of Whispering Gallery Modes (WGMs) of microsphere resonators. The coupler is made by fusion-splicing an optical fiber with a capillary tube and consequently etching the capillary wall to a thickness of a few microns. Light is coupled through the peripheral contact between inserted microsphere and the etched capillary wall. The coupling efficiency as a function of the wall thickness was studied experimentally. WGM resonance with a Q-factor of 1.14 × 10(4) was observed using a borosilicate glass microsphere with a diameter of 71 μm. The coupler operates in the reflection mode and provides a robust mechanical support to the microsphere resonator. It is expected that the new coupler may find broad applications in sensors, optical filters and lasers.

Electromagnon Resonance at Room Temperature with Gigantic Magnetochromism

NASA Astrophysics Data System (ADS)

Shishikura, H.; Tokunaga, Y.; Takahashi, Y.; Masuda, R.; Taguchi, Y.; Kaneko, Y.; Tokura, Y.

2018-04-01

The elementary excitation characteristic of magnetoelectric (ME) multiferroics is a magnon endowed with electric activity, which is referred to as an electromagnon. The electromagnon resonance mediated by the bilinear exchange coupling potentially exhibits strong terahertz light-matter interaction with optical properties different from the conventional magnon excitation. Here we report the robust electromagnon resonance on helimagnetic Y -type hexaferrites in a wide temperature range including room temperature. Furthermore, the efficient magnetic field controls of the electromagnon are demonstrated on the flexible spin structure of these compounds, leading to the generation or annihilation of the resonance as well as the large resonance energy shift. These terahertz characteristics of the electromagnon exemplify the versatile magneto-optical functionality driven by the ME coupling in multiferroics, paving a way for possible terahertz applications as well as terahertz control of a magnetic state of matter.

Nuclear spin circular dichroism.

PubMed

Vaara, Juha; Rizzo, Antonio; Kauczor, Joanna; Norman, Patrick; Coriani, Sonia

2014-04-07

Recent years have witnessed a growing interest in magneto-optic spectroscopy techniques that use nuclear magnetization as the source of the magnetic field. Here we present a formulation of magnetic circular dichroism (CD) due to magnetically polarized nuclei, nuclear spin-induced CD (NSCD), in molecules. The NSCD ellipticity and nuclear spin-induced optical rotation (NSOR) angle correspond to the real and imaginary parts, respectively, of (complex) quadratic response functions involving the dynamic second-order interaction of the electron system with the linearly polarized light beam, as well as the static magnetic hyperfine interaction. Using the complex polarization propagator framework, NSCD and NSOR signals are obtained at frequencies in the vicinity of optical excitations. Hartree-Fock and density-functional theory calculations on relatively small model systems, ethene, benzene, and 1,4-benzoquinone, demonstrate the feasibility of the method for obtaining relatively strong nuclear spin-induced ellipticity and optical rotation signals. Comparison of the proton and carbon-13 signals of ethanol reveals that these resonant phenomena facilitate chemical resolution between non-equivalent nuclei in magneto-optic spectra.

Spin-orbit excitations and electronic structure of the putative Kitaev magnet α -RuCl3

NASA Astrophysics Data System (ADS)

Sandilands, Luke J.; Tian, Yao; Reijnders, Anjan A.; Kim, Heung-Sik; Plumb, K. W.; Kim, Young-June; Kee, Hae-Young; Burch, Kenneth S.

2016-02-01

Mott insulators with strong spin-orbit coupling have been proposed to host unconventional magnetic states, including the Kitaev quantum spin liquid. The 4 d system α -RuCl3 has recently come into view as a candidate Kitaev system, with evidence for unusual spin excitations in magnetic scattering experiments. We apply a combination of optical spectroscopy and Raman scattering to study the electronic structure of this material. Our measurements reveal a series of orbital excitations involving localized total angular momentum states of the Ru ion, implying that strong spin-orbit coupling and electron-electron interactions coexist in this material. Analysis of these features allows us to estimate the spin-orbit coupling strength, as well as other parameters describing the local electronic structure, revealing a well-defined hierarchy of energy scales within the Ru d states. By comparing our experimental results with density functional theory calculations, we also clarify the overall features of the optical response. Our results demonstrate that α -RuCl3 is an ideal material system to study spin-orbit coupled magnetism on the honeycomb lattice.

Optical modulation of quantum cascade laser with optimized excitation wavelength.

PubMed

Yang, Tao; Chen, Gang; Tian, Chao; Martini, Rainer

2013-04-15

The excitation wavelength for all-optical modulation of a 10.6 μm mid-infrared (MIR) quantum cascade laser (QCL) was varied in order to obtain maximum modulation depth. Both amplitude and wavelength modulation experiments were conducted at 820 nm and 1550 nm excitation respectively, whereby the latter matches the interband transition in the QCL active region. Experimental results show that for continuous-wave mode-operated QCL, the efficiency of free carrier generation is doubled under 1550 nm excitation compared with 820 nm excitation, resulting in an increase of the amplitude modulation index from 19% to 36%. At the same time, the maximum wavelength shift is more than doubled from 1.05 nm to 2.80 nm. Furthermore, for the first time to our knowledge, we demonstrated the optical switching of a QCL operated in pulse mode by simple variation of the excitation wavelength.

Optogenetics-enabled assessment of viral gene and cell therapy for restoration of cardiac excitability

PubMed Central

Ambrosi, Christina M.; Boyle, Patrick M.; Chen, Kay; Trayanova, Natalia A.; Entcheva, Emilia

2015-01-01

Multiple cardiac pathologies are accompanied by loss of tissue excitability, which leads to a range of heart rhythm disorders (arrhythmias). In addition to electronic device therapy (i.e. implantable pacemakers and cardioverter/defibrillators), biological approaches have recently been explored to restore pacemaking ability and to correct conduction slowing in the heart by delivering excitatory ion channels or ion channel agonists. Using optogenetics as a tool to selectively interrogate only cells transduced to produce an exogenous excitatory ion current, we experimentally and computationally quantify the efficiency of such biological approaches in rescuing cardiac excitability as a function of the mode of application (viral gene delivery or cell delivery) and the geometry of the transduced region (focal or spatially-distributed). We demonstrate that for each configuration (delivery mode and spatial pattern), the optical energy needed to excite can be used to predict therapeutic efficiency of excitability restoration. Taken directly, these results can help guide optogenetic interventions for light-based control of cardiac excitation. More generally, our findings can help optimize gene therapy for restoration of cardiac excitability. PMID:26621212

Synthesis and characterization of Na(Gd0.5Lu0.5)F4: Nd3+,a core-shell free multifunctional contrast agent.

PubMed

Mimun, L Christopher; Ajithkumar, G; Rightsell, Chris; Langloss, Brian W; Therien, Michael J; Sardar, Dhiraj K

2017-02-25

Compared to conventional core-shell structures, core-shell free nanoparticles with multiple functionalities offer several advantages such as minimal synthetic complexity and low production cost. In this paper, we present the synthesis and characterization of Nd 3+ doped Na(Gd 0.5 Lu 0.5 )F 4 as a core-shell free nanoparticle system with three functionalities. Nanocrystals with 20 nm diameter, high crystallinity and a narrow particle size distributions were synthesized by the solvothermal method and characterized by various analytical techniques to understand their phase and morphology. Fluorescence characteristics under near infrared (NIR) excitation at 808 nm as well as X-ray excitation were studied to explore their potential in NIR optical and X-ray imaging. At 1.0 mol% Nd concentration, we observed a quantum yield of 25% at 1064 nm emission with 13 W/cm 2 excitation power density which is sufficiently enough for imaging applications. Under 130 kVp (5 mA) power of X-ray excitation, Nd 3+ doped Na(Gd 0.5 Lu 0.5 )F 4 shows the characteristic emission bands of Gd 3+ and Nd 3+ with the strongest emission peak at 1064 nm due to Nd 3+ . Furthermore, magnetization measurements show that the nanocrystals are paramagnetic in nature with a calculated magnetic moment per particle of ~570 μB at 2T. These preliminary results support the suitability of the present nanophosphor as a multimodal contrast agent with three imaging features viz. optical, magnetic and X-ray.

Confocal micro-Raman spectroscopy of single biological cells using optical trapping and shifted excitation difference techniques

NASA Astrophysics Data System (ADS)

Xie, Changan; Li, Yong-qing

2003-03-01

We report on the study of single biological cells with a confocal micro-Raman spectroscopy system that uses optical trapping and shifted excitation Raman difference technique. A tunable diode laser was used to capture a living cell in solution, confine it in the confocal excitation volume, and then excite the Raman scattering. The optical trapping allows us to lift the cell well off the cover plate so that the fluorescence interference from the plate can be effectively reduced. In order to further remove the interference of the fluorescence and stray light from the trapped cell, we employed a shifted excitation Raman difference technique with slightly tuned laser frequencies. With this system, high-quality Raman spectra were obtained from single optically trapped biological cells including E. coli bacteria, yeast cells, and red blood cells. A significant difference between control and heat-treated E. coli B cells was observed due to the denaturation of biomolecules.

Conceptual design of tetraazaporphyrin- and subtetraazaporphyrin-based functional nanocarbon materials: electronic structures, topologies, optical properties, and methane storage capacities.

PubMed

Belosludov, Rodion V; Rhoda, Hannah M; Zhdanov, Ravil K; Belosludov, Vladimir R; Kawazoe, Yoshiyuki; Nemykin, Victor N

2016-05-11

A large variety of conceptual three- and fourfold tetraazaporphyrin- and subtetraazaporphyrin-based functional 3D nanocage and nanobarrel structures have been proposed on the basis of in silico design. The designed structures differ in their sizes, topology, porosity, and conjugation properties. The stability of nanocages of Oh symmetry and nanobarrels of D4h symmetry was revealed on the basis of DFT and MD calculations, whereas their optical properties were assessed using a TDDFT approach and a long-range corrected LC-wPBE exchange-correlation functional. It was shown that the electronic structures and vertical excitation energies of the functional nanocage and nanobarrel structures could be easily tuned via their size, topology, and the presence of bridging sp(3) carbon atoms. TDDFT calculations suggest significantly lower excitation energies in fully conjugated nanocages and nanobarrels compared with systems with bridging sp(3) carbon fragments. Based on DFT and TDDFT calculations, the optical properties of the new materials can rival those of known quantum dots and are superior to those of monomeric phthalocyanines and their analogues. The methane gas adsorption properties of the new nanostructures and nanotubes generated by conversion from nanobarrels were studied using an MD simulation approach. The ability to store large quantities of methane (106-216 cm(3) (STP) cm(-3)) was observed in all cases with several compounds being close to or exceeding the DOE target of 180 cm(3) (STP) cm(-3) for material-based methane storage at a pressure of 3.5 MPa and room temperature.

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

Excitation of atoms and ions in plasmas by ultra-short electromagnetic pulses

NASA Astrophysics Data System (ADS)

Astapenko, V. A.; Sakhno, S. V.; Svita, S. Yu; Lisitsa, V. S.

2017-02-01

The problem of atoms and ions diagnostics in rarefied and dense plasmas by ultrashort laser pulses (USP) is under consideration. The application of USP provides: 1) excitation from ground states due to their carrier frequency high enough, 2) penetration into optically dense media due to short pulses duration. The excitation from ground atomic states increases sharply populations of excited atomic states in contrast with standard laser induced fluorescence spectroscopy based on radiative transitions between excited atomic states. New broadening parameter in radiation absorption, namely inverse pulse duration time 1/τ appears in addition to standard line-shape width in the profile G(ω). The Lyman-beta absorption spectra for USP are calculated for Holtsmark static broadening mechanism. Excitation of highly charged H-like ions in hot plasmas is described by both Gaussian shapes for Doppler broadening and pulse spectrum resulting in analytical absorption line-shape. USP penetration into optically thick media and corresponding excitation probability are calculated. It is shown a great effect of USP duration on excitation probabilities in optically thick media. The typical situations for plasma diagnostics by USP are discussed in details.

Fiber optics spectrochemical emission sensors

DOEpatents

Griffin, Jeffrey W.; Olsen, Khris B.

1992-01-01

A method of in situ monitoring of a body of a fluid stored in a tank or groundwater or vadose zone gases in a well for the presence of selected chemical species uses a probe insertable into the well or tank via a cable and having electrical apparatus for exciting selected chemical species in the body of fluid. The probe can have a pair of electrodes for initiating a spark or a plasma cell for maintaining a plasma to excite the selected chemical species. The probe also has optical apparatus for receiving optical emissions emitted by the excited species and optically transmitting the emissions via the cable to an analysis location outside the well. The analysis includes detecting a selected wavelength in the emissions indicative of the presence of the selected chemical species. A plurality of probes can be suspended at an end of a respective cable, with the transmitting and analyzing steps for each probe being synchronized sequentially for one set of support equipment and instrumentation to monitor at multiple test points. The optical apparatus is arranged about the light guide axis so that the selected chemical species are excited the fluid in alignment with the light guide axis and optical emissions are received from the excited chemical species along such axis.

Fiber optics spectrochemical emission sensors

DOEpatents

Griffin, J.W.; Olsen, K.B.

1992-02-04

A method is described of in situ monitoring of a body of a fluid stored in a tank or groundwater or vadose zone gases in a well for the presence of selected chemical species. The method uses a probe insertable into the well or tank via a cable and having an electrical apparatus for exciting selected chemical species in the body of fluid. The probe can have a pair of electrodes for initiating a spark or a plasma cell for maintaining a plasma to excite the selected chemical species. The probe also has an optical apparatus for receiving optical emissions emitted by the excited species and optically transmitting the emissions via the cable to an analysis location outside the well. The analysis includes detecting a selected wavelength in the emissions indicative of the presence of the selected chemical species. A plurality of probes can be suspended at an end of a respective cable, with the transmitting and analyzing steps for each probe being synchronized sequentially for one set of support equipment and instrumentation to monitor at multiple test points. The optical apparatus is arranged about the light guide axis so that the selected chemical species are excited in the fluid in alignment with the light guide axis. Optical emissions are received from the excited chemical species along such axis. 18 figs.

Challenges in Optical Emission Spectroscopy

NASA Astrophysics Data System (ADS)

Siepa, Sarah; Berger, Birk; Schulze, Julian; Schuengel, Edmund; von Keudell, Achim

2016-09-01

Collisional-radiative models (CRMs) are widely used to investigate plasma properties such as electron density, electron temperature and the form of the electron energy distribution function. In this work an extensive CRM for argon is presented, which models 30 excited states and various kinds of processes including electron impact excitation/de-excitation, radiation and radiation trapping. The CRM is evaluated in several test cases, i.e. inductively and capacitively coupled plasmas at various pressures, powers/voltages and gas admixtures. Deviations are found between modelled and measured spectra. The escape factor as a means of describing radiation trapping is discussed as well as the cross section data for electron impact processes. This work was supported by the Ruhr University Research School PLUS, funded by Germany's Excellence Initiative [DFG GSC 98/3].

Invited Review Article: Pump-probe microscopy.

PubMed

Fischer, Martin C; Wilson, Jesse W; Robles, Francisco E; Warren, Warren S

2016-03-01

Multiphoton microscopy has rapidly gained popularity in biomedical imaging and materials science because of its ability to provide three-dimensional images at high spatial and temporal resolution even in optically scattering environments. Currently the majority of commercial and home-built devices are based on two-photon fluorescence and harmonic generation contrast. These two contrast mechanisms are relatively easy to measure but can access only a limited range of endogenous targets. Recent developments in fast laser pulse generation, pulse shaping, and detection technology have made accessible a wide range of optical contrasts that utilize multiple pulses of different colors. Molecular excitation with multiple pulses offers a large number of adjustable parameters. For example, in two-pulse pump-probe microscopy, one can vary the wavelength of each excitation pulse, the detection wavelength, the timing between the excitation pulses, and the detection gating window after excitation. Such a large parameter space can provide much greater molecular specificity than existing single-color techniques and allow for structural and functional imaging without the need for exogenous dyes and labels, which might interfere with the system under study. In this review, we provide a tutorial overview, covering principles of pump-probe microscopy and experimental setup, challenges associated with signal detection and data processing, and an overview of applications.

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

Fischer, Martin C., E-mail: Martin.Fischer@duke.edu; Wilson, Jesse W.; Robles, Francisco E.

Multiphoton microscopy has rapidly gained popularity in biomedical imaging and materials science because of its ability to provide three-dimensional images at high spatial and temporal resolution even in optically scattering environments. Currently the majority of commercial and home-built devices are based on two-photon fluorescence and harmonic generation contrast. These two contrast mechanisms are relatively easy to measure but can access only a limited range of endogenous targets. Recent developments in fast laser pulse generation, pulse shaping, and detection technology have made accessible a wide range of optical contrasts that utilize multiple pulses of different colors. Molecular excitation with multiple pulsesmore » offers a large number of adjustable parameters. For example, in two-pulse pump-probe microscopy, one can vary the wavelength of each excitation pulse, the detection wavelength, the timing between the excitation pulses, and the detection gating window after excitation. Such a large parameter space can provide much greater molecular specificity than existing single-color techniques and allow for structural and functional imaging without the need for exogenous dyes and labels, which might interfere with the system under study. In this review, we provide a tutorial overview, covering principles of pump-probe microscopy and experimental setup, challenges associated with signal detection and data processing, and an overview of applications.« less

Invited Review Article: Pump-probe microscopy

PubMed Central

Wilson, Jesse W.; Robles, Francisco E.; Warren, Warren S.

2016-01-01

Multiphoton microscopy has rapidly gained popularity in biomedical imaging and materials science because of its ability to provide three-dimensional images at high spatial and temporal resolution even in optically scattering environments. Currently the majority of commercial and home-built devices are based on two-photon fluorescence and harmonic generation contrast. These two contrast mechanisms are relatively easy to measure but can access only a limited range of endogenous targets. Recent developments in fast laser pulse generation, pulse shaping, and detection technology have made accessible a wide range of optical contrasts that utilize multiple pulses of different colors. Molecular excitation with multiple pulses offers a large number of adjustable parameters. For example, in two-pulse pump-probe microscopy, one can vary the wavelength of each excitation pulse, the detection wavelength, the timing between the excitation pulses, and the detection gating window after excitation. Such a large parameter space can provide much greater molecular specificity than existing single-color techniques and allow for structural and functional imaging without the need for exogenous dyes and labels, which might interfere with the system under study. In this review, we provide a tutorial overview, covering principles of pump-probe microscopy and experimental setup, challenges associated with signal detection and data processing, and an overview of applications. PMID:27036751

Access to long-term optical memories using photon echoes retrieved from semiconductor spins

NASA Astrophysics Data System (ADS)

Langer, L.; Poltavtsev, S. V.; Yugova, I. A.; Salewski, M.; Yakovlev, D. R.; Karczewski, G.; Wojtowicz, T.; Akimov, I. A.; Bayer, M.

2014-11-01

The ability to store optical information is important for both classical and quantum communication. Achieving this in a comprehensive manner (converting the optical field into material excitation, storing this excitation, and releasing it after a controllable time delay) is greatly complicated by the many, often conflicting, properties of the material. More specifically, optical resonances in semiconductor quantum structures with high oscillator strength are inevitably characterized by short excitation lifetimes (and, therefore, short optical memory). Here, we present a new experimental approach to stimulated photon echoes by transferring the information contained in the optical field into a spin system, where it is decoupled from the optical vacuum field and may persist much longer. We demonstrate this for an n-doped CdTe/(Cd,Mg)Te quantum well, the storage time of which could be increased by more than three orders of magnitude, from the picosecond range up to tens of nanoseconds.

Valley-Selective Exciton Bistability in a Suspended Monolayer Semiconductor.

PubMed

Xie, Hongchao; Jiang, Shengwei; Shan, Jie; Mak, Kin Fai

2018-05-09

We demonstrate robust optical bistability, the phenomenon of two well-discriminated stable states depending upon the history of the optical input, in fully suspended monolayers of WSe 2 at low temperatures near the exciton resonance. Optical bistability has been achieved under continuous-wave optical excitation that is red-detuned from the exciton resonance at an intensity level of 10 3 W/cm 2 . The observed bistability is originated from a photothermal mechanism, which provides both optical nonlinearity and passive feedback, two essential elements for optical bistability. The low thermal conductance of suspended samples is primarily responsible for the low excitation intensities required for optical bistability. Under a finite out-of-plane magnetic field, the exciton bistability becomes helicity dependent due to the exciton valley Zeeman effect, which enables repeatable switching of the sample reflectance by light polarization. Our study has opened up exciting opportunities in controlling light with light, including its wavelength, power, and polarization, using monolayer semiconductors.

Controlling the excited-state dynamics of low band gap, near-infrared absorbers via proquinoidal unit electronic structural modulation

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

Bai, Yusong; Rawson, Jeff; Roget, Sean A.

While the influence of proquinoidal character upon the linear absorption spectrum of low optical bandgap π-conjugated polymers and molecules is well understood, its impact upon excited-state relaxation pathways and dynamics remains obscure. We report the syntheses, electronic structural properties, and excited-state dynamics of a series of model highly conjugated near-infrared (NIR)-absorbing chromophores based on a (porphinato)metal(II)-proquinoidal spacer-(porphinato)metal(II) (PM-Sp-PM) structural motif. A combination of excited-state dynamical studies and time-dependent density functional theory calculations: (i) points to the cardinal role that excited-state configuration interaction (CI) plays in determining the magnitudes of S 1 → S 0 radiative (k r), S 1 → T 1 intersystem crossing (k ISC), and S 1 → S 0 internal conversion (k IC) rate constants in these PM-Sp-PM chromophores, and (ii) suggests that a primary determinant of CI magnitude derives from the energetic alignment of the PM and Sp fragment LUMOs (ΔE L). These insights not only enable steering of excited-state relaxation dynamics of high oscillator strength NIR absorbers to realize either substantial fluorescence or long-lived triplets (τmore » $$_ {T_1}$$ > μs) generated at unit quantum yield (Φ ISC = 100%), but also crafting of those having counter-intuitive properties: for example, while (porphinato)platinum compounds are well known to generate non-emissive triplet states (Φ ISC = 100%) upon optical excitation at ambient temperature, diminishing the extent of excited-state CI in these systems realizes long-wavelength absorbing heavy-metal fluorophores. In conclusion, this work highlights approaches to: (i) modulate low-lying singlet excited-state lifetime over the picosecond-to-nanosecond time domain, (ii) achieve NIR fluorescence with quantum yields up to 25%, (iii) tune the magnitude of S 1–T 1 ISC rate constant from 10 9 to 10 12 s -1 and (iv) realize T 1-state lifetimes that range from ~0.1 to several μs, for these model PM-Sp-PM chromophores, and renders new insights to evolve bespoke photophysical properties for low optical bandgap π-conjugated polymers and molecules based on proquinoidal conjugation motifs.« less

Controlling the excited-state dynamics of low band gap, near-infrared absorbers via proquinoidal unit electronic structural modulation

DOE PAGES

Bai, Yusong; Rawson, Jeff; Roget, Sean A.; ...

2017-06-07

While the influence of proquinoidal character upon the linear absorption spectrum of low optical bandgap π-conjugated polymers and molecules is well understood, its impact upon excited-state relaxation pathways and dynamics remains obscure. We report the syntheses, electronic structural properties, and excited-state dynamics of a series of model highly conjugated near-infrared (NIR)-absorbing chromophores based on a (porphinato)metal(II)-proquinoidal spacer-(porphinato)metal(II) (PM-Sp-PM) structural motif. A combination of excited-state dynamical studies and time-dependent density functional theory calculations: (i) points to the cardinal role that excited-state configuration interaction (CI) plays in determining the magnitudes of S 1 → S 0 radiative (k r), S 1 → T 1 intersystem crossing (k ISC), and S 1 → S 0 internal conversion (k IC) rate constants in these PM-Sp-PM chromophores, and (ii) suggests that a primary determinant of CI magnitude derives from the energetic alignment of the PM and Sp fragment LUMOs (ΔE L). These insights not only enable steering of excited-state relaxation dynamics of high oscillator strength NIR absorbers to realize either substantial fluorescence or long-lived triplets (τmore » $$_ {T_1}$$ > μs) generated at unit quantum yield (Φ ISC = 100%), but also crafting of those having counter-intuitive properties: for example, while (porphinato)platinum compounds are well known to generate non-emissive triplet states (Φ ISC = 100%) upon optical excitation at ambient temperature, diminishing the extent of excited-state CI in these systems realizes long-wavelength absorbing heavy-metal fluorophores. In conclusion, this work highlights approaches to: (i) modulate low-lying singlet excited-state lifetime over the picosecond-to-nanosecond time domain, (ii) achieve NIR fluorescence with quantum yields up to 25%, (iii) tune the magnitude of S 1–T 1 ISC rate constant from 10 9 to 10 12 s -1 and (iv) realize T 1-state lifetimes that range from ~0.1 to several μs, for these model PM-Sp-PM chromophores, and renders new insights to evolve bespoke photophysical properties for low optical bandgap π-conjugated polymers and molecules based on proquinoidal conjugation motifs.« less

Ultrafast Silicon Photonics with Visible to Mid-Infrared Pumping of Silicon Nanocrystals.

PubMed

Diroll, Benjamin T; Schramke, Katelyn S; Guo, Peijun; Kortshagen, Uwe R; Schaller, Richard D

2017-10-11

Dynamic optical control of infrared (IR) transparency and refractive index is achieved using boron-doped silicon nanocrystals excited with mid-IR optical pulses. Unlike previous silicon-based optical switches, large changes in transmittance are achieved without a fabricated structure by exploiting strong light coupling of the localized surface plasmon resonance (LSPR) produced from free holes of p-type silicon nanocrystals. The choice of optical excitation wavelength allows for selectivity between hole heating and carrier generation through intraband or interband photoexcitation, respectively. Mid-IR optical pumping heats the free holes of p-Si nanocrystals to effective temperatures greater than 3500 K. Increases of the hole effective mass at high effective hole temperatures lead to a subpicosecond change of the dielectric function, resulting in a redshift of the LSPR, modulating mid-IR transmission by as much as 27%, and increasing the index of refraction by more than 0.1 in the mid-IR. Low hole heat capacity dictates subpicosecond hole cooling, substantially faster than carrier recombination, and negligible heating of the Si lattice, permitting mid-IR optical switching at terahertz repetition frequencies. Further, the energetic distribution of holes at high effective temperatures partially reverses the Burstein-Moss effect, permitting the modulation of transmittance at telecommunications wavelengths. The results presented here show that doped silicon, particularly in micro- or nanostructures, is a promising dynamic metamaterial for ultrafast IR photonics.

Ultrafast Silicon Photonics with Visible to Mid-Infrared Pumping of Silicon Nanocrystals

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

Diroll, Benjamin T.; Schramke, Katelyn S.; Guo, Peijun

Dynamic optical control of infrared (IR) transparency and refractive index is achieved using boron-doped silicon nanocrystals excited with mid-IR optical pulses. Also, unlike previous silicon-based optical switches, large changes in transmittance are achieved without a fabricated structure by exploiting strong light coupling of the localized surface plasmon resonance (LSPR) produced from free holes of p-type silicon nanocrystals. The choice of optical excitation wavelength allows selectivity between hole heating and carrier generation through intraband or interband photoexcitation, respectively. Mid-IR optical pumping heats the free holes of p-Si nanocrystals to effective temperatures greater than 3500 K. Increases of the hole effective massmore » at high effective hole temperatures lead to a sub-picosecond change of the dielectric function resulting in a redshift of the LSPR, modulating mid-IR transmission by as much as 27% and increasing the index of refraction by more than 0.1 in the mid-IR. Low hole heat capacity dictates sub-picosecond hole cooling, substantially faster than carrier recombination, and negligible heating of the Si lattice, permitting mid-IR optical switching at terahertz repetition frequencies. Further, the energetic distribution of holes at high effective temperatures partially reverses the Burstein-Moss effect, permitting modulation of transmittance at telecommunications wavelengths. Lastly, the results presented here show that doped silicon, particularly in micro- or nanostructures, is a promising dynamic metamaterial for ultrafast IR photonics.« less

Ultrafast Silicon Photonics with Visible to Mid-Infrared Pumping of Silicon Nanocrystals

DOE PAGES

Diroll, Benjamin T.; Schramke, Katelyn S.; Guo, Peijun; ...

2017-09-11

Dynamic optical control of infrared (IR) transparency and refractive index is achieved using boron-doped silicon nanocrystals excited with mid-IR optical pulses. Also, unlike previous silicon-based optical switches, large changes in transmittance are achieved without a fabricated structure by exploiting strong light coupling of the localized surface plasmon resonance (LSPR) produced from free holes of p-type silicon nanocrystals. The choice of optical excitation wavelength allows selectivity between hole heating and carrier generation through intraband or interband photoexcitation, respectively. Mid-IR optical pumping heats the free holes of p-Si nanocrystals to effective temperatures greater than 3500 K. Increases of the hole effective massmore » at high effective hole temperatures lead to a sub-picosecond change of the dielectric function resulting in a redshift of the LSPR, modulating mid-IR transmission by as much as 27% and increasing the index of refraction by more than 0.1 in the mid-IR. Low hole heat capacity dictates sub-picosecond hole cooling, substantially faster than carrier recombination, and negligible heating of the Si lattice, permitting mid-IR optical switching at terahertz repetition frequencies. Further, the energetic distribution of holes at high effective temperatures partially reverses the Burstein-Moss effect, permitting modulation of transmittance at telecommunications wavelengths. Lastly, the results presented here show that doped silicon, particularly in micro- or nanostructures, is a promising dynamic metamaterial for ultrafast IR photonics.« less

Valence and charge-transfer optical properties for some SinCm (m, n ≤ 12) clusters: Comparing TD-DFT, complete-basis-limit EOMCC, and benchmarks from spectroscopy

NASA Astrophysics Data System (ADS)

Lutz, Jesse J.; Duan, Xiaofeng F.; Ranasinghe, Duminda S.; Jin, Yifan; Margraf, Johannes T.; Perera, Ajith; Burggraf, Larry W.; Bartlett, Rodney J.

2018-05-01

Accurate optical characterization of the closo-Si12C12 molecule is important to guide experimental efforts toward the synthesis of nano-wires, cyclic nano-arrays, and related array structures, which are anticipated to be robust and efficient exciton materials for opto-electronic devices. Working toward calibrated methods for the description of closo-Si12C12 oligomers, various electronic structure approaches are evaluated for their ability to reproduce measured optical transitions of the SiC2, Si2Cn (n = 1-3), and Si3Cn (n = 1, 2) clusters reported earlier by Steglich and Maier [Astrophys. J. 801, 119 (2015)]. Complete-basis-limit equation-of-motion coupled-cluster (EOMCC) results are presented and a comparison is made between perturbative and renormalized non-iterative triples corrections. The effect of adding a renormalized correction for quadruples is also tested. Benchmark test sets derived from both measurement and high-level EOMCC calculations are then used to evaluate the performance of a variety of density functionals within the time-dependent density functional theory (TD-DFT) framework. The best-performing functionals are subsequently applied to predict valence TD-DFT excitation energies for the lowest-energy isomers of SinC and Sin-1C7-n (n = 4-6). TD-DFT approaches are then applied to the SinCn (n = 4-12) clusters and unique spectroscopic signatures of closo-Si12C12 are discussed. Finally, various long-range corrected density functionals, including those from the CAM-QTP family, are applied to a charge-transfer excitation in a cyclic (Si4C4)4 oligomer. Approaches for gauging the extent of charge-transfer character are also tested and EOMCC results are used to benchmark functionals and make recommendations.

Tip-enhanced near-field optical microscopy

PubMed Central

Mauser, Nina; Hartschuh, Achim

2013-01-01

Tip-enhanced near-field optical microscopy (TENOM) is a scanning probe technique capable of providing a broad range of spectroscopic information on single objects and structured surfaces at nanometer spatial resolution and with highest detection sensitivity. In this review, we first illustrate the physical principle of TENOM that utilizes the antenna function of a sharp probe to efficiently couple light to excitations on nanometer length scales. We then discuss the antenna-induced enhancement of different optical sample responses including Raman scattering, fluorescence, generation of photocurrent and electroluminescence. Different experimental realizations are presented and several recent examples that demonstrate the capabilities of the technique are reviewed. PMID:24100541

Electron Transport and Nonlinear Optical Properties of Substituted Aryldimesityl Boranes: A DFT Study

PubMed Central

Pandith, Altaf Hussain; Islam, Nasarul

2014-01-01

A comprehensive theoretical study was carried out on a series of aryldimesityl borane (DMB) derivatives using Density Functional theory. Optimized geometries and electronic parameters like electron affinity, reorganization energy, frontiers molecular contours, polarizability and hyperpolarizability have been calculated by employing B3PW91/6-311++G (d, p) level of theory. Our results show that the Hammett function and geometrical parameters correlates well with the reorganization energies and hyperpolarizability for the series of DMB derivatives studied in this work. The orbital energy study reveals that the electron releasing substituents increase the LUMO energies and electron withdrawing substituents decrease the LUMO energies, reflecting the electron transport character of aryldimesityl borane derivatives. From frontier molecular orbitals diagram it is evident that mesityl rings act as the donor, while the phenylene and Boron atom appear as acceptors in these systems. The calculated hyperpolarizability of secondary amine derivative of DMB is 40 times higher than DMB (1). The electronic excitation contributions to the hyperpolarizability studied by using TDDFT calculation shows that hyperpolarizability correlates well with dipole moment in ground and excited state and excitation energy in terms of the two-level model. Thus the results of these calculations can be helpful in designing the DMB derivatives for efficient electron transport and nonlinear optical material by appropriate substitution with electron releasing or withdrawing substituents on phenyl ring of DMB system. PMID:25479382

Wiring up pre-characterized single-photon emitters by laser lithography

NASA Astrophysics Data System (ADS)

Shi, Q.; Sontheimer, B.; Nikolay, N.; Schell, A. W.; Fischer, J.; Naber, A.; Benson, O.; Wegener, M.

2016-08-01

Future quantum optical chips will likely be hybrid in nature and include many single-photon emitters, waveguides, filters, as well as single-photon detectors. Here, we introduce a scalable optical localization-selection-lithography procedure for wiring up a large number of single-photon emitters via polymeric photonic wire bonds in three dimensions. First, we localize and characterize nitrogen vacancies in nanodiamonds inside a solid photoresist exhibiting low background fluorescence. Next, without intermediate steps and using the same optical instrument, we perform aligned three-dimensional laser lithography. As a proof of concept, we design, fabricate, and characterize three-dimensional functional waveguide elements on an optical chip. Each element consists of one single-photon emitter centered in a crossed-arc waveguide configuration, allowing for integrated optical excitation and efficient background suppression at the same time.

Influence of optical pumping wavelength on the ultrafast gain and phase recovery acceleration of quantum-dot semiconductor optical amplifiers

NASA Astrophysics Data System (ADS)

Kim, Jungho

2013-10-01

We numerically investigate the influence of the optical pumping wavelength on the ultrafast gain and phase recovery acceleration of quantum-dot (QD) semiconductor optical amplifiers (SOAs) by solving 1088 coupled rate equations. The temporal variations of the gain and phase recovery response at the ground state (GS) of QDs are calculated at various signal wavelengths when the optical pumping wavelengths at the excited state (ES) of QDs are varied. The phase recovery response is fastest when the wavelength of the signal and pumping beams corresponds to the respective emission wavelength of the GS and the ES in the same size of QDs. The absorption efficiency of the optical pumping beam at the ES is determined by the Lorentzian line shape function of the homogeneous broadening.

Detection, Evaluation, and Optimization of Optical Signals Generated by Fiber Optic Bragg Gratings Under Dynamic Excitations

NASA Technical Reports Server (NTRS)

Adamovsky, Grigory; Lekki, John; Lock, James A.

2002-01-01

The dynamic response of a fiber optic Bragg grating to mechanical vibrations is examined both theoretically and experimentally. The theoretical expressions describing the consequences of changes in the grating's reflection spectrum are derived for partially coherent beams in an interferometer. The analysis is given in terms of the dominant wavelength, optical bandwidth, and optical path difference of the interfering signals. Changes in the reflection spectrum caused by a periodic stretching and compression of the grating were experimentally measured using an unbalanced Michelson interferometer, a Michelson interferometer with a non-zero optical path difference. The interferometer's sensitivity to changes in dominant wavelength of the interfering beams was measured as a function of interferometer unbalance and was compared to theoretical predictions. The theoretical analysis enables the user to determine the optimum performance for an unbalanced interferometer.

2D XAFS-XEOL Spectroscopy - Some recent developments

NASA Astrophysics Data System (ADS)

Ward, M. J.; Smith, J. G.; Regier, T. Z.; Sham, T. K.

2013-03-01

The use of optical photons to measure the modulation of the absorption coefficient upon X-ray excitation, or optical XAFS, is of particular interest for application to the study of light emitting semiconducting nanomaterials due to the additional information that may be gained. The potential for site-selectivity, elemental and excitation energy specific luminescence decay channels, and surface vs. bulk effects all make the use of X-ray excited optical luminescence (XEOL) desirable as a detection method. Previous experiments have made use of a monochromator to select the optical emission wavelength used to monitor optical XAFS. This method of detection suffers from the primary limitation of only being able to monitor the optical response at one emission wavelength. By combining the high resolution soft X-ray Spherical Grating Monochromator beam-line at the Canadian Light Source with an Ocean Optics QE 65000 fast CCD spectrophotometer and custom integration software we have developed a technique for collecting 2D XAFS-XEOL spectra, in which the excitation energy is scanned and a XEOL spectra is collected for every energy value. Herein we report the development of this technique and its capabilities using the study of the luminescence emitted from single crystal zinc oxide as an example.

Excitation spectra of aromatic molecules within a real-space G W -BSE formalism: Role of self-consistency and vertex corrections

DOE PAGES

Hung, Linda; da Jornada, Felipe H.; Souto-Casares, Jaime; ...

2016-08-15

Here, we present first-principles calculations on the vertical ionization potentials (IPs), electron affinities (EAs), and singlet excitation energies on an aromatic-molecule test set (benzene, thiophene, 1,2,5-thiadiazole, naphthalene, benzothiazole, and tetrathiafulvalene) within the GW and Bethe-Salpeter equation (BSE) formalisms. Our computational framework, which employs a real-space basis for ground-state and a transition-space basis for excited-state calculations, is well suited for high-accuracy calculations on molecules, as we show by comparing against G0W0 calculations within a plane-wave-basis formalism. We then generalize our framework to test variants of the GW approximation that include a local density approximation (LDA)–derived vertex function (Γ LDA ) andmore » quasiparticle-self-consistent (QS) iterations. We find that Γ LDA and quasiparticle self-consistency shift IPs and EAs by roughly the same magnitude, but with opposite sign for IPs and the same sign for EAs. G0W0 and QS GWΓ LDA are more accurate for IPs, while G 0W 0Γ LDA and QS GW are best for EAs. For optical excitations, we find that perturbative GW-BSE underestimates the singlet excitation energy, while self-consistent GW-BSE results in good agreement with previous best-estimate values for both valence and Rydberg excitations. Finally, our work suggests that a hybrid approach, in which G0W0 energies are used for occupied orbitals and G0W0Γ LDA for unoccupied orbitals, also yields optical excitation energies in good agreement with experiment but at a smaller computational cost.« less

Excitation spectra of aromatic molecules within a real-space G W -BSE formalism: Role of self-consistency and vertex corrections

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

Hung, Linda; da Jornada, Felipe H.; Souto-Casares, Jaime

Here, we present first-principles calculations on the vertical ionization potentials (IPs), electron affinities (EAs), and singlet excitation energies on an aromatic-molecule test set (benzene, thiophene, 1,2,5-thiadiazole, naphthalene, benzothiazole, and tetrathiafulvalene) within the GW and Bethe-Salpeter equation (BSE) formalisms. Our computational framework, which employs a real-space basis for ground-state and a transition-space basis for excited-state calculations, is well suited for high-accuracy calculations on molecules, as we show by comparing against G0W0 calculations within a plane-wave-basis formalism. We then generalize our framework to test variants of the GW approximation that include a local density approximation (LDA)–derived vertex function (Γ LDA ) andmore » quasiparticle-self-consistent (QS) iterations. We find that Γ LDA and quasiparticle self-consistency shift IPs and EAs by roughly the same magnitude, but with opposite sign for IPs and the same sign for EAs. G0W0 and QS GWΓ LDA are more accurate for IPs, while G 0W 0Γ LDA and QS GW are best for EAs. For optical excitations, we find that perturbative GW-BSE underestimates the singlet excitation energy, while self-consistent GW-BSE results in good agreement with previous best-estimate values for both valence and Rydberg excitations. Finally, our work suggests that a hybrid approach, in which G0W0 energies are used for occupied orbitals and G0W0Γ LDA for unoccupied orbitals, also yields optical excitation energies in good agreement with experiment but at a smaller computational cost.« less

Surface-modified TiO2 powders with phenol derivatives: A comparative DFT and experimental study

NASA Astrophysics Data System (ADS)

Sredojević, Dušan N.; Kovač, Tijana; Džunuzović, Enis; Ðorđević, Vesna; Grgur, Branimir N.; Nedeljković, Jovan M.

2017-10-01

The charge transfer complex formation between TiO2 powder and variety of phenol derivatives (phenol, 4-nitrophenol, 4-bromophenol, 4-tert-butylphenol, hydroquinone) was achieved. The red-shift of optical absorption was observed upon surface modification of TiO2 powders with phenol derivatives. The influence of substituent functional groups in para position on the optical band gap and conduction band edge of inorganic/organic hybrids was studied using reflection spectroscopy and cyclic voltammetry. The experimental findings were supported by density functional theory calculations. The measured reflection spectra of surface-modified TiO2 powders with phenol derivatives were compared with calculated electronic excitation spectra of corresponding model systems.

Three-photon Gaussian-Gaussian-Laguerre-Gaussian excitation of a localized atom to a highly excited Rydberg state

NASA Astrophysics Data System (ADS)

Mashhadi, L.

2017-12-01

Optical vortices are currently one of the most intensively studied topics in light-matter interaction. In this work, a three-step axial Doppler- and recoil-free Gaussian-Gaussian-Laguerre-Gaussian (GGLG) excitation of a localized atom to the highly excited Rydberg state is presented. By assuming a large detuning for intermediate states, an effective quadrupole excitation related to the Laguerre-Gaussian (LG) excitation to the highly excited Rydberg state is obtained. This special excitation system radially confines the single highly excited Rydberg atom independently of the trapping system into a sharp potential landscape into the so-called ‘far-off-resonance optical dipole-quadrupole trap’ (FORDQT). The key parameters of the Rydberg excitation to the highly excited state, namely the effective Rabi frequency and the effective detuning including a position-dependent AC Stark shift, are calculated in terms of the basic parameters of the LG beam and of the polarization of the excitation lasers. It is shown that the obtained parameters can be tuned to have a precise excitation of a single atom to the desired Rydberg state as well. The features of transferring the optical orbital and spin angular momentum of the polarized LG beam to the atom via quadrupole Rydberg excitation offer a long-lived and controllable qudit quantum memory. In addition, in contrast to the Gaussian laser beam, the doughnut-shaped LG beam makes it possible to use a high intensity laser beam to increase the signal-to-noise ratio in quadrupole excitation with minimized perturbations coming from stray light broadening in the last Rydberg excitation process.

Ultrahigh resolution multicolor colocalization of single fluorescent probes

DOEpatents

Weiss, Shimon; Michalet, Xavier; Lacoste, Thilo D.

2005-01-18

A novel optical ruler based on ultrahigh-resolution colocalization of single fluorescent probes is described. Two unique families of fluorophores are used, namely energy-transfer fluorescent beads and semiconductor nanocrystal (NC) quantum dots, that can be excited by a single laser wavelength but emit at different wavelengths. A novel multicolor sample-scanning confocal microscope was constructed which allows one to image each fluorescent light emitter, free of chromatic aberrations, by scanning the sample with nanometer scale steps using a piezo-scanner. The resulting spots are accurately localized by fitting them to the known shape of the excitation point-spread-function of the microscope.

Coherent electron{endash}hole correlations in quantum dots

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

Joensson, L.; Steiner, M.M.; Wilkins, J.W.

1997-03-01

Using numerical time propagation of the electron{endash}hole wave function, we demonstrate how various coherent correlation effects can be observed by laser excitation of a nanoscale semiconductor quantum dot. The lowest-lying states of an electron{endash}hole pair, when appropriately excited by a laser pulse, give rise to charge oscillations that are manifested by beatings in the optical or intraband polarizations. A GaAs 5{times}25{times}25 nm{sup 3} dot in the effective-mass approximation, including the screened Coulomb interaction between the electron and a heavy or light hole, is simulated. {copyright} {ital 1997 American Institute of Physics.}

Exciton-polariton dynamics in a GaAs bulk microcavity

NASA Astrophysics Data System (ADS)

Ceccherini, S.; Gurioli, M.; Bogani, F.; Colocci, M.; Tredicucci, A.; Bassani, F.; Beltram, F.; Sorba, L.

1998-01-01

We present a full analysis of exciton dynamics in a GaAs λ/2 bulk microcavity following excitation by ultrafast laser pulses. Coherent dynamics was probed by means of an interferometric technique; beating and dephasing times were studied for various excitation intensities. At high incident power, population effects begin to show up reducing exciton oscillator strength and suppressing Rabi splitting. This feature produces marked non-linearities in the input-output characteristic of the optical functions, which were studied in view of reaching bistable operation. Theoretical calculations performed within the transfer-matrix framework show good agreement with experimental results.

Image-guided urologic surgery: intraoperative optical imaging and tissue interrogation (Conference Presentation)

NASA Astrophysics Data System (ADS)

Liao, Joseph C.

2017-02-01

Emerging optical imaging technologies can be integrated in the operating room environment during minimally invasive and open urologic surgery, including oncologic surgery of the bladder, prostate, and kidney. These technologies include macroscopic fluorescence imaging that provides contrast enhancement between normal and diseased tissue and microscopic imaging that provides tissue characterization. Optical imaging technologies that have reached the clinical arena in urologic surgery are reviewed, including photodynamic diagnosis, near infrared fluorescence imaging, optical coherence tomography, and confocal laser endomicroscopy. Molecular imaging represents an exciting future arena in conjugating cancer-specific contrast agents to fluorophores to improve the specificity of disease detection. Ongoing efforts are underway to translate optimal targeting agents and imaging modalities, with the goal to improve cancer-specific and functional outcomes.

On the analysis of para-ammonia observations

NASA Technical Reports Server (NTRS)

Kuiper, T. B. H.

1994-01-01

The intensities and optical depths of the (1, 1), (2, 2), and (2, 1) inversion transitions of ammonia can be calculated quite accurately without solving the equations of statistical equilibrium. A two-temperature partition function suffices. The excitation of the K-ladders can be approximated by using a temperature obtained from a two-level model with the (2, 1) and (1, 1) levels. Distribution of populations between the ladders is described with the kinetic temperature. This enables one to compute the (1, 1) and (2, 1) inversion transition excitation temperatures and optical depths. To compute the (2, 2) brightness temperatures, the fractional population of the (2, 2) doublet is computed from the population of the (1, 1) doublet using the 'true rotation temperature,' which is calculated using a three-level model with the (2, 1), (2, 2), and (1, 1) levels. In spite of some iterative steps, the calculation is quite fast.

Optical properties of voltage sensitive hemicyanine dyes of variable hydrophobicity confined within surfactant micelles

NASA Astrophysics Data System (ADS)

Naeem, Kashif; Naseem, Bushra; Shah, S. S.; Shah, Syed W. H.

2017-11-01

The optical properties of amphiphilic hemicyanine dyes with variable hydrophobicity, confined within anionic micelles of sodium dodecylbenzenesulfonate (NaDDBS) have been studied by UV-visible absorption spectroscopy. The confinement constant, K conf has been determined for each entrapped dye. The ion-pair formation between dye and surfactant causes a decline in electronic transition energy (ΔE T) when dye alkyl chains are smaller due to stabilization of both the ground and excited state. ΔE T values gradually increase with increase in dye hydrophobicity that hampers the electrostatic interaction with dialkylammonium moiety and consequently excited state stabilization is compromised. The average number of dye molecules trapped in a single micelle was also determined. The negative values of Gibbs free energy indicate that the dye entrapment within micelles is energetically favored. These findings have significance for developing functional materials with peculiar luminescent properties, especially for more effective probing of complex biological systems.

Dynamical multiferroicity

NASA Astrophysics Data System (ADS)

Juraschek, Dominik M.; Fechner, Michael; Balatsky, Alexander V.; Spaldin, Nicola A.

2017-06-01

An appealing mechanism for inducing multiferroicity in materials is the generation of electric polarization by a spatially varying magnetization that is coupled to the lattice through the spin-orbit interaction. Here we describe the reciprocal effect, in which a time-dependent electric polarization induces magnetization even in materials with no existing spin structure. We develop a formalism for this dynamical multiferroic effect in the case for which the polarization derives from optical phonons, and compute the strength of the phonon Zeeman effect, which is the solid-state equivalent of the well-established vibrational Zeeman effect in molecules, using density functional theory. We further show that a recently observed behavior—the resonant excitation of a magnon by optically driven phonons—is described by the formalism. Finally, we discuss examples of scenarios that are not driven by lattice dynamics and interpret the excitation of Dzyaloshinskii-Moriya-type electromagnons and the inverse Faraday effect from the viewpoint of dynamical multiferroicity.

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.

Spin Flips versus Spin Transport in Nonthermal Electrons Excited by Ultrashort Optical Pulses in Transition Metals

NASA Astrophysics Data System (ADS)

Shokeen, V.; Sanchez Piaia, M.; Bigot, J.-Y.; Müller, T.; Elliott, P.; Dewhurst, J. K.; Sharma, S.; Gross, E. K. U.

2017-09-01

A joint theoretical and experimental investigation is performed to understand the underlying physics of laser-induced demagnetization in Ni and Co films with varying thicknesses excited by 10 fs optical pulses. Experimentally, the dynamics of spins is studied by determining the time-dependent amplitude of the Voigt vector, retrieved from a full set of magnetic and nonmagnetic quantities performed on both sides of films, with absolute time reference. Theoretically, ab initio calculations are performed using time-dependent density functional theory. Overall, we demonstrate that spin-orbit induced spin flips are the most significant contributors with superdiffusive spin transport, which assumes only that the transport of majority spins without spin flips induced by scattering does not apply in Ni. In Co it plays a significant role during the first ˜20 fs only. Our study highlights the material dependent nature of the demagnetization during the process of thermalization of nonequilibrium spins.

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.

Spectral asymmetry of atoms in the van der Waals potential of an optical nanofiber

NASA Astrophysics Data System (ADS)

Patterson, B. D.; Solano, P.; Julienne, P. S.; Orozco, L. A.; Rolston, S. L.

2018-03-01

We measure the modification of the transmission spectra of cold 87Rb atoms in the proximity of an optical nanofiber (ONF). Van der Waals interactions between the atoms an the ONF surface decrease the resonance frequency of atoms closer to the surface. An asymmetric spectra of the atoms holds information of their spatial distribution around the ONF. We use a far-detuned laser beam coupled to the ONF to thermally excite atoms at the ONF surface. We study the change of transmission spectrum of these atoms as a function of heating laser power. A semiclassical phenomenological model for the thermal excitation of atoms in the atom-surface van der Waals bound states is in good agreement with the measurements. This result suggests that van der Waals potentials could be used to trap and probe atoms at few nanometers from a dielectric surface, a key tool for hybrid photonic-atomic quantum systems.

Transient Melting and Recrystallization of Semiconductor Nanocrystals Under Multiple Electron–Hole Pair Excitation

DOE PAGES

Kirschner, Matthew S.; Hannah, Daniel C.; Diroll, Benjamin T.; ...

2017-07-28

Ultrafast optical pump, X-ray diffraction probe experiments were performed on CdSe nanocrystal (NC) colloidal dispersions as functions of particle size, polytype, and pump fluence. Bragg peak shifts relate heating and peak amplitude reduction confers lattice disordering. For smaller NCs, melting initiates upon absorption of as few as ~15 electron-hole pair excitations per NC on average (0.89 excitations/nm 3 for a 1.5-nm radius) with roughly the same excitation density inducing melting for all examined NCs. Diffraction intensity recovery kinetics, attributable to recrystallization, occur over hundreds of picoseconds with slower recoveries for larger particles. Zincblende and wurtzite NCs revert to initial structuresmore » following intense photoexcitation suggesting melting occurs primarily at the surface, as supported by simulations. Electronic structure calculations relate significant band gap narrowing with decreased crystallinity. Here, these findings reflect the need to consider the physical stability of nanomaterials and related electronic impacts in high intensity excitation applications such as lasing and solid-state lighting.« less

Transient Melting and Recrystallization of Semiconductor Nanocrystals Under Multiple Electron–Hole Pair Excitation

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

Kirschner, Matthew S.; Hannah, Daniel C.; Diroll, Benjamin T.

Ultrafast optical pump, X-ray diffraction probe experiments were performed on CdSe nanocrystal (NC) colloidal dispersions as functions of particle size, polytype, and pump fluence. Bragg peak shifts relate heating and peak amplitude reduction confers lattice disordering. For smaller NCs, melting initiates upon absorption of as few as ~15 electron-hole pair excitations per NC on average (0.89 excitations/nm 3 for a 1.5-nm radius) with roughly the same excitation density inducing melting for all examined NCs. Diffraction intensity recovery kinetics, attributable to recrystallization, occur over hundreds of picoseconds with slower recoveries for larger particles. Zincblende and wurtzite NCs revert to initial structuresmore » following intense photoexcitation suggesting melting occurs primarily at the surface, as supported by simulations. Electronic structure calculations relate significant band gap narrowing with decreased crystallinity. Here, these findings reflect the need to consider the physical stability of nanomaterials and related electronic impacts in high intensity excitation applications such as lasing and solid-state lighting.« less

Transient Melting and Recrystallization of Semiconductor Nanocrystals Under Multiple Electron-Hole Pair Excitation.

PubMed

Kirschner, Matthew S; Hannah, Daniel C; Diroll, Benjamin T; Zhang, Xiaoyi; Wagner, Michael J; Hayes, Dugan; Chang, Angela Y; Rowland, Clare E; Lethiec, Clotilde M; Schatz, George C; Chen, Lin X; Schaller, Richard D

2017-09-13

Ultrafast optical pump, X-ray diffraction probe experiments were performed on CdSe nanocrystal (NC) colloidal dispersions as functions of particle size, polytype, and pump fluence. Bragg peak shifts related to heating and peak amplitude reduction associated with lattice disordering are observed. For smaller NCs, melting initiates upon absorption of as few as ∼15 electron-hole pair excitations per NC on average (0.89 excitations/nm 3 for a 1.5 nm radius) with roughly the same excitation density inducing melting for all examined NCs. Diffraction intensity recovery kinetics, attributable to recrystallization, occur over hundreds of picoseconds with slower recoveries for larger particles. Zincblende and wurtzite NCs revert to initial structures following intense photoexcitation suggesting melting occurs primarily at the surface, as supported by simulations. Electronic structure calculations relate significant band gap narrowing with decreased crystallinity. These findings reflect the need to consider the physical stability of nanomaterials and related electronic impacts in high intensity excitation applications such as lasing and solid-state lighting.

Observation of organ-pipe acoustic excitations in supported thin films

NASA Astrophysics Data System (ADS)

Zhang, X.; Sooryakumar, R.; Every, A. G.; Manghnani, M. H.

2001-08-01

Brillouin light scattering from supported silicon oxynitride films reveal an extended series of acoustic excitations occurring at regular frequency intervals when the mode wave vector is perpendicular to the film surface. These periodic peaks are identified as distinct standing wave excitations that, similar to harmonics of an open-ended organ pipe, occur due to the boundary conditions imposed by the free surface and substrate-film interface. The surface ripple and volume elasto-optic scattering mechanisms contribute to the scattering cross sections and lead to dramatic interference effects at low frequencies where the surface corrugations play a dominant role. The transformation of these standing wave excitations to modes with finite in-plane wave vectors is also investigated. The results are discussed in the framework of a Green's-function formalism that reproduces the experimental features and illustrate the importance of the standing modes in evaluating the longitudinal elastic properties of the films.

Comparison of vapor formation of water at the solid/water interface to colloidal solutions using optically excited gold nanostructures.

PubMed

Baral, Susil; Green, Andrew J; Livshits, Maksim Y; Govorov, Alexander O; Richardson, Hugh H

2014-02-25

The phase transformation properties of liquid water to vapor is characterized by optical excitation of the lithographically fabricated single gold nanowrenches and contrasted to the phase transformation properties of gold nanoparticles located and optically excited in a bulk solution system [two and three dimensions]. The 532 nm continuous wave excitation of a single gold nanowrench results in superheating of the water to the spinodal decomposition temperature of 580 ± 20 K with bubble formation below the spinodal decomposition temperature being a rare event. Between the spinodal decomposition temperature and the boiling point liquid water is trapped into a metastable state because a barrier to vapor nucleation exists that must be overcome before the thermodynamically stable state is realized. The phase transformation for an optically heated single gold nanowrench is different from the phase transformation of optically excited colloidal gold nanoparticles solution where collective heating effects dominates and leads to the boiling of the solution exactly at the boiling point. In the solution case, the optically excited ensemble of nanoparticles collectively raises the ambient temperature of water to the boiling point where liquid is converted into vapor. The striking difference in the boiling properties of the single gold nanowrench and the nanoparticle solution system can be explained in terms of the vapor-nucleation mechanism, the volume of the overheated liquid, and the collective heating effect. The interpretation of the observed regimes of heating and vaporization is consistent with our theoretical modeling. In particular, we explain with our theory why the boiling with the collective heating in a solution requires 3 orders of magnitude less intensity compared to the case of optically driven single nanowrench.

Method and apparatus for imaging a sample on a device

DOEpatents

Trulson, Mark; Stern, David; Fiekowsky, Peter; Rava, Richard; Walton, Ian; Fodor, Stephen P. A.

1996-01-01

The present invention provides methods and systems for detecting a labeled marker on a sample located on a support. The imaging system comprises a body for immobilizing the support, an excitation radiation source and excitation optics to generate and direct the excitation radiation at the sample. In response, labeled material on the sample emits radiation which has a wavelength that is different from the excitation wavelength, which radiation is collected by collection optics and imaged onto a detector which generates an image of the sample.

Full-field modal analysis during base motion excitation using high-speed 3D digital image correlation

NASA Astrophysics Data System (ADS)

Molina-Viedma, Ángel J.; López-Alba, Elías; Felipe-Sesé, Luis; Díaz, Francisco A.

2017-10-01

In recent years, many efforts have been made to exploit full-field measurement optical techniques for modal identification. Three-dimensional digital image correlation using high-speed cameras has been extensively employed for this purpose. Modal identification algorithms are applied to process the frequency response functions (FRF), which relate the displacement response of the structure to the excitation force. However, one of the most common tests for modal analysis involves the base motion excitation of a structural element instead of force excitation. In this case, the relationship between response and excitation is typically based on displacements, which are known as transmissibility functions. In this study, a methodology for experimental modal analysis using high-speed 3D digital image correlation and base motion excitation tests is proposed. In particular, a cantilever beam was excited from its base with a random signal, using a clamped edge join. Full-field transmissibility functions were obtained through the beam and converted into FRF for proper identification, considering a single degree-of-freedom theoretical conversion. Subsequently, modal identification was performed using a circle-fit approach. The proposed methodology facilitates the management of the typically large amounts of data points involved in the DIC measurement during modal identification. Moreover, it was possible to determine the natural frequencies, damping ratios and full-field mode shapes without requiring any additional tests. Finally, the results were experimentally validated by comparing them with those obtained by employing traditional accelerometers, analytical models and finite element method analyses. The comparison was performed by using the quantitative indicator modal assurance criterion. The results showed a high level of correspondence, consolidating the proposed experimental methodology.

[Development of a Surgical Navigation System with Beam Split and Fusion of the Visible and Near-Infrared Fluorescence].

PubMed

Yang, Xiaofeng; Wu, Wei; Wang, Guoan

2015-04-01

This paper presents a surgical optical navigation system with non-invasive, real-time, and positioning characteristics for open surgical procedure. The design was based on the principle of near-infrared fluorescence molecular imaging. The in vivo fluorescence excitation technology, multi-channel spectral camera technology and image fusion software technology were used. Visible and near-infrared light ring LED excitation source, multi-channel band pass filters, spectral camera 2 CCD optical sensor technology and computer systems were integrated, and, as a result, a new surgical optical navigation system was successfully developed. When the near-infrared fluorescence was injected, the system could display anatomical images of the tissue surface and near-infrared fluorescent functional images of surgical field simultaneously. The system can identify the lymphatic vessels, lymph node, tumor edge which doctor cannot find out with naked eye intra-operatively. Our research will guide effectively the surgeon to remove the tumor tissue to improve significantly the success rate of surgery. The technologies have obtained a national patent, with patent No. ZI. 2011 1 0292374. 1.

Spectral broadening of optical transitions in InAs/GaAs coupled quantum dot pairs

NASA Astrophysics Data System (ADS)

Kumar, P.; Czarnocki, C.; Jennings, C.; Casara, J.; Monteros, A. L.; Zahbihi, N.; Scheibner, M.; Economou, S. E.; Bracker, A. S.; Pursley, B. C.; Gammon, D.; Carter, S. G.

The optical transitions in InAs/GaAs coupled quantum dot (CQD) pairs are investigated experimentally. These coupled dot systems provide new means to study the interaction of quantum states with the mechanical modes of the crystal environment. Here, the line width and line shape of CQD optical transitions are analyzed in detail as a function of temperature, excitation power, excitation energy, and tunnel coupling strength. A significant line broadening, up to 25 times the typical lifetime-limited linewidth of single-dot excitons, is being observed at level anti-crossings where the coherent tunnel coupling between spatially direct and indirect exciton states is considerable. The experimental observations are compared with theoretical predictions where linewidth broadening at anti-crossings is attributed to the phonon assisted transitions, and found to be strongly dependent on the energy splitting of the two exciton branches. This work focuses on understanding the linewidth broadening due to the pure dephasing, and fundamental aspects of the interaction of these systems with the local environment. This work was supported by the Defense Threat Reduction Agency, Basic Research Award HDTRA1-15-1-0011.

Influence of image charge effect on impurity-related optical absorption coefficients and refractive index changes in a spherical quantum dot

NASA Astrophysics Data System (ADS)

Vartanian, A. L.; Asatryan, A. L.; Vardanyan, L. A.

2017-03-01

We have investigated the influence of an image charge effect (ICE) on the energies of the ground and first few excited states of a hydrogen-like impurity in a spherical quantum dot (QD) in the presence of an external electric field. The oscillator strengths of transitions from the 1 s -like state to excited states of 2px and 2pz symmetries are calculated as the functions of the strengths of the confinement potential and the electric field. Also, we have studied the effect of image charges on linear and third-order nonlinear optical absorption coefficients and refractive index changes (RICs). The results show that image charges lead to the decrease of energies for all the hydrogen-like states, to the significant enhancement of the oscillator strengths of transitions between the impurity states, and to comparatively large blue shifts in linear, nonlinear, and total absorption coefficients and refractive index changes. Our results indicate that the total optical characteristics can be controlled by the strength of the confinement and the electric field.

Two-photon voltage imaging using a genetically encoded voltage indicator

PubMed Central

Akemann, Walther; Sasaki, Mari; Mutoh, Hiroki; Imamura, Takeshi; Honkura, Naoki; Knöpfel, Thomas

2013-01-01

Voltage-sensitive fluorescent proteins (VSFPs) are a family of genetically-encoded voltage indicators (GEVIs) reporting membrane voltage fluctuation from genetically-targeted cells in cell cultures to whole brains in awake mice as demonstrated earlier using 1-photon (1P) fluorescence excitation imaging. However, in-vivo 1P imaging captures optical signals only from superficial layers and does not optically resolve single neurons. Two-photon excitation (2P) imaging, on the other hand, has not yet been convincingly applied to GEVI experiments. Here we show that 2P imaging of VSFP Butterfly 1.2 expresssing pyramidal neurons in layer 2/3 reports optical membrane voltage in brain slices consistent with 1P imaging but with a 2–3 larger ΔR/R value. 2P imaging of mouse cortex in-vivo achieved cellular resolution throughout layer 2/3. In somatosensory cortex we recorded sensory responses to single whisker deflections in anesthetized mice at full frame video rate. Our results demonstrate the feasibility of GEVI-based functional 2P imaging in mouse cortex. PMID:23868559

Fabrication of bright and thin Zn₂SiO₄ luminescent film for electron beam excitation-assisted optical microscope.

PubMed

Furukawa, Taichi; Kanamori, Satoshi; Fukuta, Masahiro; Nawa, Yasunori; Kominami, Hiroko; Nakanishi, Yoichiro; Sugita, Atsushi; Inami, Wataru; Kawata, Yoshimasa

2015-07-13

We fabricated a bright and thin Zn₂SiO₄ luminescent film to serve as a nanometric light source for high-spatial-resolution optical microscopy based on electron beam excitation. The Zn₂SiO₄ luminescent thin film was fabricated by annealing a ZnO film on a Si₃N₄ substrate at 1000 °C in N₂. The annealed film emitted bright cathodoluminescence compared with the as-deposited film. The film is promising for nano-imaging with electron beam excitation-assisted optical microscopy. We evaluated the spatial resolution of a microscope developed using this Zn₂SiO₄ luminescent thin film. This is the first report of the investigation and application of ZnO/Si₃N₄ annealed at a high temperature (1000 °C). The fabricated Zn₂SiO₄ film is expected to enable high-frame-rate dynamic observation with ultra-high resolution using our electron beam excitation-assisted optical microscopy.

Fiber-optic apparatus and method for measurement of luminescence and raman scattering

DOEpatents

Myrick, Michael L.; Angel, Stanley M.

1993-01-01

A dual fiber forward scattering optrode for Raman spectroscopy with the remote ends of the fibers in opposed, spaced relationship to each other to form a analyte sampling space therebetween and the method of measuring Raman spectra utilizing same. One optical fiber is for sending an exciting signal to the remote sampling space and, at its remote end, has a collimating microlens and an optical filter for filtering out background emissions generated in the fiber. The other optical fiber is for collecting the Raman scattering signal at the remote sampling space and, at its remote end, has a collimating microlens and an optical filter to prevent the exciting signal from the exciting fiber from entering the collection fiber and to thereby prevent the generation of background emissions in the collecting fiber.

Absolute measurements of the triplet-triplet annihilation rate and the charge-carrier recombination layer thickness in working polymer light-emitting diodes based on polyspirobifluorene

NASA Astrophysics Data System (ADS)

Rothe, C.; Al Attar, H. A.; Monkman, A. P.

2005-10-01

The triplet exciton densities in electroluminescent devices prepared from two polyspirobifluorene derivatives have been investigated by means of time-resolved transient triplet absorption as a function of optical and electrical excitation power at 20 K. Because of the low mobility of the triplet excitons at this temperature, the triplet generation profile within the active polymer layer is preserved throughout the triplet lifetime and as a consequence the absolute triplet-triplet annihilation efficiency is not homogeneously distributed but depends on position within the active layer. This then gives a method to measure the charge-carrier recombination layer after electrical excitation relative to the light penetration depth, which is identical to the triplet generation layer after optical excitation. With the latter being obtained from ellipsometry, an absolute value of 5 nm is found for the exciton formation layer in polyspirobifluorene devices. This layer increases to 11 nm if the balance between the electron and the hole mobility is improved by chemically modifying the polymer backbone. Also, and consistent with previous work, triplet diffusion is dispersive at low temperature. As a consequence of this, the triplet-triplet annihilation rate is not a constant in the classical sense but depends on the triplet excitation dose. At 20 K and for typical excitation doses, absolute values of the latter rate are of the order of 10-14cm3s-1 .

Wave excitations of drifting two-dimensional electron gas under strong inelastic scattering

NASA Astrophysics Data System (ADS)

Korotyeyev, V. V.; Kochelap, V. A.; Varani, L.

2012-10-01

We have analyzed low-temperature behavior of two-dimensional electron gas in polar heterostructures subjected to a high electric field. When the optical phonon emission is the fastest relaxation process, we have found existence of collective wave-like excitations of the electrons. These wave-like excitations are periodic in time oscillations of the electrons in both real and momentum spaces. The excitation spectra are of multi-branch character with considerable spatial dispersion. There are one acoustic-type and a number of optical-type branches of the spectra. Their small damping is caused by quasi-elastic scattering of the electrons and formation of relevant space charge. Also there exist waves with zero frequency and finite spatial periods—the standing waves. The found excitations of the electron gas can be interpreted as synchronous in time and real space manifestation of well-known optical-phonon-transient-time-resonance. Estimates of parameters of the excitations for two polar heterostructures, GaN/AlGaN and ZnO/MgZnO, have shown that excitation frequencies are in THz-frequency range, while standing wave periods are in sub-micrometer region.

A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions

DOE PAGES

Wu, Guanhong; Zhou, Chenkun; Ming, Wenmei; ...

2018-05-23

Organic–inorganic metal halide hybrids have emerged as a new class of materials with fascinating optical and electronic properties. The exceptional structure tunability has enabled the development of materials with various dimensionalities at the molecular level, from three-dimensional (3D) to 2D, 1D, and 0D. Here, we report a new 1D lead chloride hybrid, C 4N 2H 14PbCl 4, which exhibits unusual inverse excitation-dependent broadband emission from bluish-green to yellow. Density functional theory calculations were performed to better understand the mechanism of this excitation-dependent broadband emission. This 1D hybrid material is found to have two emission centers, corresponding to the self-trapped excitonsmore » (STEs) and vacancy-bound excitons. The excitation-dependent emission is due to different populations of these two types of excitons generated at different excitation wavelengths. Furthermore, this work shows the rich chemistry and physics of organic–inorganic metal halide hybrids and paves the way to achieving novel light emitters with excitation-dependent broadband emissions at room temperature.« less

A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions

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

Wu, Guanhong; Zhou, Chenkun; Ming, Wenmei

Organic–inorganic metal halide hybrids have emerged as a new class of materials with fascinating optical and electronic properties. The exceptional structure tunability has enabled the development of materials with various dimensionalities at the molecular level, from three-dimensional (3D) to 2D, 1D, and 0D. Here, we report a new 1D lead chloride hybrid, C 4N 2H 14PbCl 4, which exhibits unusual inverse excitation-dependent broadband emission from bluish-green to yellow. Density functional theory calculations were performed to better understand the mechanism of this excitation-dependent broadband emission. This 1D hybrid material is found to have two emission centers, corresponding to the self-trapped excitonsmore » (STEs) and vacancy-bound excitons. The excitation-dependent emission is due to different populations of these two types of excitons generated at different excitation wavelengths. Furthermore, this work shows the rich chemistry and physics of organic–inorganic metal halide hybrids and paves the way to achieving novel light emitters with excitation-dependent broadband emissions at room temperature.« less

Optical Mapping of Membrane Potential and Epicardial Deformation in Beating Hearts.

PubMed

Zhang, Hanyu; Iijima, Kenichi; Huang, Jian; Walcott, Gregory P; Rogers, Jack M

2016-07-26

Cardiac optical mapping uses potentiometric fluorescent dyes to image membrane potential (Vm). An important limitation of conventional optical mapping is that contraction is usually arrested pharmacologically to prevent motion artifacts from obscuring Vm signals. However, these agents may alter electrophysiology, and by abolishing contraction, also prevent optical mapping from being used to study coupling between electrical and mechanical function. Here, we present a method to simultaneously map Vm and epicardial contraction in the beating heart. Isolated perfused swine hearts were stained with di-4-ANEPPS and fiducial markers were glued to the epicardium for motion tracking. The heart was imaged at 750 Hz with a video camera. Fluorescence was excited with cyan or blue LEDs on alternating camera frames, thus providing a 375-Hz effective sampling rate. Marker tracking enabled the pixel(s) imaging any epicardial site within the marked region to be identified in each camera frame. Cyan- and blue-elicited fluorescence have different sensitivities to Vm, but other signal features, primarily motion artifacts, are common. Thus, taking the ratio of fluorescence emitted by a motion-tracked epicardial site in adjacent frames removes artifacts, leaving Vm (excitation ratiometry). Reconstructed Vm signals were validated by comparison to monophasic action potentials and to conventional optical mapping signals. Binocular imaging with additional video cameras enabled marker motion to be tracked in three dimensions. From these data, epicardial deformation during the cardiac cycle was quantified by computing finite strain fields. We show that the method can simultaneously map Vm and strain in a left-sided working heart preparation and can image changes in both electrical and mechanical function 5 min after the induction of regional ischemia. By allowing high-resolution optical mapping in the absence of electromechanical uncoupling agents, the method relieves a long-standing limitation of optical mapping and has potential to enhance new studies in coupled cardiac electromechanics. Copyright © 2016 Biophysical Society. Published by Elsevier Inc. All rights reserved.

Absorption and fluorescence spectra of heterocyclic isomers from long-range-corrected density functional theory in polarizable continuum approach.

PubMed

Kityk, Andriy V

2012-03-22

Long-range-corrected (LC) DFT/TDDFT methods may provide adequate description of ground and excited state properties; however, accuracy of such an approach depends much on a range separation (exchange screening) representing adjustable model parameter. Its relation to a size or specific of molecular systems has been explored in numerous studies, whereas the effect of solvent environment is usually ignored during the evaluation of state properties. To benchmark and assess the quality of the LC-DFT/TDDFT formalism, we report the optical absorption and fluorescence emission energies of organic heterocyclic isomers, DPIPQ and PTNA, calculated by LC-BLYP DFT/TDDFT method in the polarizable continuum (PCM) approach. The calculations are compared with the optical absorption and fluorescence spectra measured in organic solvents of different polarity. Despite a considerable structural difference, both dyes exhibit quite similar range separations being somewhat different for the optical absorption and fluorescence emission processes. Properly parametrized LC-BLYP xc-potential well reproduces basic features of the optical absorption spectra including the electronic transitions to higher excited states. The DFT/TDDFT/PCM analysis correctly predicts the solvation trends although solvatochromic shifts of the electronic transition energies appear to be evidently underestimated in most cases, especially for the fluorescence emission. Considering the discrepancy between the experiment and theory, evaluated state dipole moments and solvation corrections to the exchange screening are analyzed. The results of the present study emphasize the importance of a solvent-dependent range separation in DFT/TDDFT/PCM calculations for investigating excited state properties. © 2012 American Chemical Society

Luminescent rare earth vanadate nanoparticles doped with Eu3+ and Bi3 for sensing and imaging applications

NASA Astrophysics Data System (ADS)

Escudero, Alberto; Carrillo-Carrión, Carolina; Zyuzin, Mikhail; Hartmann, Raimo; Ashraf, Sumaira; Parak, Wolfgang J.

2016-03-01

Nanoparticles (NPs) are attracting interest in nanomedicine due to their potential medical applications, ranging from optical biolabels and contrast agents for magnetic resonance imaging to carriers for drug and gene delivery for disease therapy.[1] Rare earth (RE) based nanophosphors exhibit important advantages compared with other available luminescent materials, such as quantum dots and nanostructures functionalized with organic dyes, due to their lower toxicities, photostabilities, high thermal and chemical stabilities, high luminescence quantum yields, and sharp emission bands.[2] Yttrium orthovanadate NPs doped with Eu3+ and Bi3+, functionalized with poly acryl acid (PAA), and excitable by near-ultraviolet light have been synthesized by homogeneous precipitation at 120 °C from solutions of rare earth precursors (yttrium acetylacetonate and europium nitrate), bismuth nitrate, sodium orthovanadate, and PAA, in an ethylene glycol/water mixture. Quasispheres with sizes from 93 to 51 nm were obtained. The as synthesized NPs were already functionalized with PAA. The NPs showed the typical red luminescence of Eu3+, which can be excited with near-UV light through an energy transfer from the vanadate anion. The presence of Bi3+ shifts the maximum of the broad excitation band from 280 nm to 342 nm. This excitation path is much more efficient than the direct excitation of the Eu3+ electronic levels, and results in a much higher luminescence. The NPs can be uptaken by HeLa cells, and are eventually located in the lysosomes after being internalized. Finally, the functionalization with PAA provides -COOH anchors for adding functional ligands of biomedical interest that can be used for sensing applications.

Multi-quantum excitation in optically pumped alkali atom: rare gas mixtures

NASA Astrophysics Data System (ADS)

Galbally-Kinney, K. L.; Rawlins, W. T.; Davis, S. J.

2014-03-01

Diode-pumped alkali laser (DPAL) technology offers a means of achieving high-energy gas laser output through optical pumping of the D-lines of Cs, Rb, and K. The exciplex effect, based on weak attractive forces between alkali atoms and polarizable rare gas atoms (Ar, Kr, Xe), provides an alternative approach via broadband excitation of exciplex precursors (XPAL). In XPAL configurations, we have observed multi-quantum excitation within the alkali manifolds which result in infrared emission lines between 1 and 4 μm. The observed excited states include the 42FJ states of both Cs and Rb, which are well above the two-photon energy of the excitation laser in each case. We have observed fluorescence from multi-quantum states for excitation wavelengths throughout the exciplex absorption bands of Cs-Ar, Cs-Kr, and Cs-Xe. The intensity scaling is roughly first-order or less in both pump power and alkali concentration, suggesting a collisional energy pooling excitation mechanism. Collisional up-pumping appears to present a parasitic loss term for optically pumped atomic systems at high intensities, however there may also be excitation of other lasing transitions at infrared wavelengths.

Instability of superfluid Fermi gases induced by a rotonlike density mode in optical lattices

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

Yunomae, Yoshihiro; Yamamoto, Daisuke; Danshita, Ippei

2009-12-15

We study the stability of superfluid Fermi gases in deep optical lattices in the BCS-Bose-Einstein condensation (BEC) crossover at zero temperature. Within the tight-binding attractive Hubbard model, we calculate the spectrum of the low-energy Anderson-Bogoliubov (AB) mode as well as the single-particle excitations in the presence of superfluid flow in order to determine the critical velocities. To obtain the spectrum of the AB mode, we calculate the density response function in the generalized random-phase approximation applying the Green's function formalism developed by Cote and Griffin to the Hubbard model. We find that the spectrum of the AB mode is separatedmore » from the particle-hole continuum having the characteristic rotonlike minimum at short wavelength due to the strong charge-density-wave fluctuations. The energy of the rotonlike minimum decreases with increasing the lattice velocity and it reaches zero at the critical velocity which is smaller than the pair-breaking velocity. This indicates that the superfluid state is energetically unstable due to the spontaneous emission of the short-wavelength rotonlike excitations of the AB mode instead due to pair breaking. We determine the critical velocities as functions of the interaction strength across the BCS-BEC crossover regime.« less

How To Identify Plasmons from the Optical Response of Nanostructures

PubMed Central

2017-01-01

A promising trend in plasmonics involves shrinking the size of plasmon-supporting structures down to a few nanometers, thus enabling control over light–matter interaction at extreme-subwavelength scales. In this limit, quantum mechanical effects, such as nonlocal screening and size quantization, strongly affect the plasmonic response, rendering it substantially different from classical predictions. For very small clusters and molecules, collective plasmonic modes are hard to distinguish from other excitations such as single-electron transitions. Using rigorous quantum mechanical computational techniques for a wide variety of physical systems, we describe how an optical resonance of a nanostructure can be classified as either plasmonic or nonplasmonic. More precisely, we define a universal metric for such classification, the generalized plasmonicity index (GPI), which can be straightforwardly implemented in any computational electronic-structure method or classical electromagnetic approach to discriminate plasmons from single-particle excitations and photonic modes. Using the GPI, we investigate the plasmonicity of optical resonances in a wide range of systems including: the emergence of plasmonic behavior in small jellium spheres as the size and the number of electrons increase; atomic-scale metallic clusters as a function of the number of atoms; and nanostructured graphene as a function of size and doping down to the molecular plasmons in polycyclic aromatic hydrocarbons. Our study provides a rigorous foundation for the further development of ultrasmall nanostructures based on molecular plasmonics. PMID:28651057

Tunable liquid optics: electrowetting-controlled liquid mirrors based on self-assembled Janus tiles.

PubMed

Bucaro, Michael A; Kolodner, Paul R; Taylor, J Ashley; Sidorenko, Alex; Aizenberg, Joanna; Krupenkin, Tom N

2009-04-09

In this paper, we describe a tunable, high-reflectivity optofluidic device based on self-assembly of anisotropically functionalized hexagonal micromirrors (Janus tiles) on the surface of an oil droplet to create a concave liquid mirror. The liquid mirror is deposited on a patterned transparent electrode that allows the focal length and axial position to be electrically controlled. The mirror is mechanically robust and retains its integrity even at high levels of vibrational excitation of the interface. The use of reflection instead of refraction overcomes the limited available refractive-index contrast between pairs of density-matched liquids, allowing stronger focusing than is possible for a liquid lens of the same geometry. This approach is compatible with optical instruments that could provide novel functionality-for example, a dynamic 3D projector, i.e., a light source which can scan an image onto a moving, nonplanar focal surface. Janus tiles with complex optical properties can be manufactured using our approach, thus potentially enabling a wide range of novel optical elements.

Tunable liquid optics: electrowetting-controlled liquid mirrors based on self-assembled Janus tiles

NASA Astrophysics Data System (ADS)

Krupenkin, Tom; Bucaro, Mike; Kolodner, Paul; Taylor, Ashley; Sidorenko, Alex; Aizenberg, Joanna

2009-03-01

In this work we describe a tunable, high-reflectivity optofluidic device based on self-assembly of anisotropically-functionalized hexagonal micromirrors (Janus tiles) on the surface of an oil droplet to create a concave liquid mirror. The liquid mirror is deposited on a patterned transparent electrode that allows the focal length and axial position to be electrically controlled. The mirror is mechanically robust and retains its integrity even at high levels of vibrational excitation of the interface. The use of reflection instead of refraction overcomes the limited available refractive-index contrast between pairs of density-matched liquids, allowing stronger focusing than is possible for a liquid lens of the same geometry. This approach is compatible with optical instruments that could provide novel functionality - for example, a dynamic 3D projector; i.e., a light source which can scan an image onto a moving, non-planar focal surface. Janus tiles with complex optical properties can be manufactured using our approach, thus potentially enabling a wide range of novel optical elements.

FIBER AND INTEGRAL OPTICS: Mode composition of radiation in graded-index waveguides with random microbending of the axis

NASA Astrophysics Data System (ADS)

Valyaev, A. B.; Krivoshlykov, S. G.

1989-06-01

It is shown that the problem of investigating the mode composition of a partly coherent radiation beam in a randomly inhomogeneous medium can be reduced to a study of evolution of the energy of individual modes and of the coefficients of correlations between the modes. General expressions are obtained for the coupling coefficients of modes in a parabolic waveguide with a random microbending of the axis and an analysis is made of their evolution as a function of the excitation conditions. An estimate is obtained of the distance in which a steady-state energy distribution between the modes is established. Explicit expressions are obtained for the correlation function in the case when a waveguide is excited by off-axial Gaussian beams or Gauss-Hermite modes.

Designing graphene absorption in a multispectral plasmon-enhanced infrared detector

DOE PAGES

Goldflam, Michael D.; Fei, Zhe; Ruiz, Isaac; ...

2017-05-18

Here, we have examined graphene absorption in a range of graphene-based infrared devices that combine either monolayer or bilayer graphene with three different gate dielectrics. Electromagnetic simulations show that the optical absorption in graphene in these devices, an important factor in a functional graphene-based detector, is strongly dielectric-dependent. Our simulations reveal that plasmonic excitation in graphene can significantly influence the percentage of light absorbed in the entire device, as well as the graphene layer itself, with graphene absorption exceeding 25% in regions where plasmonic excitation occurs. Notably, the dielectric environment of graphene has a dramatic influence on the strength andmore » wavelength range over which the plasmons can be excited, making dielectric choice paramount to final detector tunability and sensitivity.« less

Time-dependent transition density matrix for visualizing charge-transfer excitations in photoexcited organic donor-acceptor systems

NASA Astrophysics Data System (ADS)

Li, Yonghui; Ullrich, Carsten

2013-03-01

The time-dependent transition density matrix (TDM) is a useful tool to visualize and interpret the induced charges and electron-hole coherences of excitonic processes in large molecules. Combined with time-dependent density functional theory on a real-space grid (as implemented in the octopus code), the TDM is a computationally viable visualization tool for optical excitation processes in molecules. It provides real-time maps of particles and holes which gives information on excitations, in particular those that have charge-transfer character, that cannot be obtained from the density alone. Some illustration of the TDM and comparison with standard density difference plots will be shown for photoexcited organic donor-acceptor molecules. This work is supported by NSF Grant DMR-1005651

Designing graphene absorption in a multispectral plasmon-enhanced infrared detector

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

Goldflam, Michael D.; Fei, Zhe; Ruiz, Isaac

Here, we have examined graphene absorption in a range of graphene-based infrared devices that combine either monolayer or bilayer graphene with three different gate dielectrics. Electromagnetic simulations show that the optical absorption in graphene in these devices, an important factor in a functional graphene-based detector, is strongly dielectric-dependent. Our simulations reveal that plasmonic excitation in graphene can significantly influence the percentage of light absorbed in the entire device, as well as the graphene layer itself, with graphene absorption exceeding 25% in regions where plasmonic excitation occurs. Notably, the dielectric environment of graphene has a dramatic influence on the strength andmore » wavelength range over which the plasmons can be excited, making dielectric choice paramount to final detector tunability and sensitivity.« less

Tip-enhanced near-field optical microscope with side-on and ATR-mode sample excitation for super-resolution Raman imaging of surfaces

NASA Astrophysics Data System (ADS)

Heilman, A. L.; Gordon, M. J.

2016-06-01

A tip-enhanced near-field optical microscope with side-on and attenuated total reflectance (ATR) excitation and collection is described and used to demonstrate sub-diffraction-limited (super-resolution) optical and chemical characterization of surfaces. ATR illumination is combined with an Au optical antenna tip to show that (i) the tip can quantitatively transduce the optical near-field (evanescent waves) above the surface by scattering photons into the far-field, (ii) the ATR geometry enables excitation and characterization of surface plasmon polaritons (SPPs), whose associated optical fields are shown to enhance Raman scattering from a thin layer of copper phthalocyanine (CuPc), and (iii) SPPs can be used to plasmonically excite the tip for super-resolution chemical imaging of patterned CuPc via tip-enhanced Raman spectroscopy (TERS). ATR-illumination TERS is also quantitatively compared with the more conventional side-on illumination scheme. In both cases, spatial resolution was better than 40 nm and tip on/tip off Raman enhancement factors were >6500. Furthermore, ATR illumination was shown to provide similar Raman signal levels at lower "effective" pump powers due to additional optical energy delivered by SPPs to the active region in the tip-surface gap.

Isotropically sensitive optical filter employing atomic resonance transitions

DOEpatents

Marling, J.B.

An ultra-high Q isotropically sensitive optical filter or optical detector is disclosed employing atomic resonance transitions. More specifically, atomic resonance transitions utilized in conjunction with two optical bandpass filters provide an optical detector having a wide field of view (approx. 2 ..pi.. steradians) and very narrow acceptance bandwidth approaching 0.01A. A light signal to be detected is transmitted through an outer bandpass filter into a resonantly absorbing atomic vapor, the excited atomic vapor than providing a fluorescence signal at a different wavelength which is transmitted through an inner bandpass filters have no common transmission band, therby resulting in complete blockage of all optical signals that are not resonantly shifted in wavelength by the intervening atomic vapor. Two embodiments are disclosed, one in which the light signal raises atoms contained in the atomic vapor from the ground state to an excited state from which fluorescence occurs, and the other in which a pump laser is used to raise the atoms in the ground state to a first excited state from which the light signal then is resonantly absorbed, thereby raising the atoms to a second excited state from which fluorescence occurs. A specific application is described in which an optical detector according to the present invention can be located in an orbiting satellite.

Tip-enhanced near-field optical microscope with side-on and ATR-mode sample excitation for super-resolution Raman imaging of surfaces

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

Heilman, A. L.; Gordon, M. J.

A tip-enhanced near-field optical microscope with side-on and attenuated total reflectance (ATR) excitation and collection is described and used to demonstrate sub-diffraction-limited (super-resolution) optical and chemical characterization of surfaces. ATR illumination is combined with an Au optical antenna tip to show that (i) the tip can quantitatively transduce the optical near-field (evanescent waves) above the surface by scattering photons into the far-field, (ii) the ATR geometry enables excitation and characterization of surface plasmon polaritons (SPPs), whose associated optical fields are shown to enhance Raman scattering from a thin layer of copper phthalocyanine (CuPc), and (iii) SPPs can be used tomore » plasmonically excite the tip for super-resolution chemical imaging of patterned CuPc via tip-enhanced Raman spectroscopy (TERS). ATR-illumination TERS is also quantitatively compared with the more conventional side-on illumination scheme. In both cases, spatial resolution was better than 40 nm and tip on/tip off Raman enhancement factors were >6500. Furthermore, ATR illumination was shown to provide similar Raman signal levels at lower “effective” pump powers due to additional optical energy delivered by SPPs to the active region in the tip-surface gap.« less

Holographic imaging and photostimulation of neural activity.

PubMed

Yang, Weijian; Yuste, Rafael

2018-06-01

Optical imaging methods are powerful tools in neuroscience as they can systematically monitor the activity of neuronal populations with high spatiotemporal resolution using calcium or voltage indicators. Moreover, caged compounds and optogenetic actuators enable to optically manipulate neural activity. Among optical methods, computer-generated holography offers an enormous flexibility to sculpt the excitation light in three-dimensions (3D), particularly when combined with two-photon light sources. By projecting holographic light patterns on the sample, the activity of multiple neurons across a 3D brain volume can be simultaneously imaged or optically manipulated with single-cell precision. This flexibility makes two-photon holographic microscopy an ideal all-optical platform to simultaneously read and write activity in neuronal populations in vivo in 3D, a critical ability to dissect the function of neural circuits. Copyright © 2018 Elsevier Ltd. All rights reserved.

Optical and Nonlinear Optical Response of Light Sensor Thin Films

PubMed Central

Liu, Huimin; Rua, Armando; Vasquez, Omar; Vikhnin, Valentin S.; Fernandez, Felix E.; Fonseca, Luis F.; Resto, Oscar; Weisz, Svi Z.

2005-01-01

For potential ultrafast optical sensor application, both VO2 thin films and nanocomposite crystal-Si enriched SiO2 thin films grown on fused quartz substrates were successfully prepared using pulsed laser deposition (PLD) and RF co-sputtering techniques. In photoluminescence (PL) measurement c-Si/SiO2 film contains nanoparticles of crystal Si exhibits strong red emission with the band maximum ranging from 580 to 750 nm. With ultrashort pulsed laser excitation all films show extremely intense and ultrafast nonlinear optical (NLO) response. The recorded holography from all these thin films in a degenerate-four-wave-mixing configuration shows extremely large third-order response. For VO2 thin films, an optically induced semiconductor-to-metal phase transition (PT) immediately occurred upon laser excitation. it accompanied. It turns out that the fast excited state dynamics was responsible to the induced PT. For c-Si/SiO2 film, its NLO response comes from the contribution of charge carriers created by laser excitation in conduction band of the c-Si nanoparticles. It was verified by introducing Eu3+ which is often used as a probe sensing the environment variations. It turns out that the entire excited state dynamical process associated with the creation, movement and trapping of the charge carriers has a characteristic 500 ps duration.

Development of a nonlinear fiber-optic spectrometer for human lung tissue exploration

PubMed Central

Peyrot, Donald A.; Lefort, Claire; Steffenhagen, Marie; Mansuryan, Tigran; Ducourthial, Guillaume; Abi-Haidar, Darine; Sandeau, Nicolas; Vever-Bizet, Christine; Kruglik, Sergei G.; Thiberville, Luc; Louradour, Frédéric; Bourg-Heckly, Geneviève

2012-01-01

Several major lung pathologies are characterized by early modifications of the extracellular matrix (ECM) fibrillar collagen and elastin network. We report here the development of a nonlinear fiber-optic spectrometer, compatible with an endoscopic use, primarily intended for the recording of second-harmonic generation (SHG) signal of collagen and two-photon excited fluorescence (2PEF) of both collagen and elastin. Fiber dispersion is accurately compensated by the use of a specific grism-pair stretcher, allowing laser pulse temporal width around 70 fs and excitation wavelength tunability from 790 to 900 nm. This spectrometer was used to investigate the excitation wavelength dependence (from 800 to 870 nm) of SHG and 2PEF spectra originating from ex vivo human lung tissue samples. The results were compared with spectral responses of collagen gel and elastin powder reference samples and also with data obtained using standard nonlinear microspectroscopy. The excitation-wavelength-tunable nonlinear fiber-optic spectrometer presented in this study allows performing nonlinear spectroscopy of human lung tissue ECM through the elastin 2PEF and the collagen SHG signals. This work opens the way to tunable excitation nonlinear endomicroscopy based on both distal scanning of a single optical fiber and proximal scanning of a fiber-optic bundle. PMID:22567579

Isotropically sensitive optical filter employing atomic resonance transitions

DOEpatents

Marling, John B.

1981-01-01

An ultra-high Q isotropically sensitive optical filter or optical detector employing atomic resonance transitions. More specifically, atomic resonance transitions utilized in conjunction with two optical bandpass filters provide an optical detector having a wide field of view (.about.2.pi. steradians) and very narrow acceptance bandwidth approaching 0.01 A. A light signal to be detected is transmitted through an outer bandpass filter into a resonantly absorbing atomic vapor, the excited atomic vapor then providing a fluorescence signal at a different wavelength which is transmitted through an inner bandpass filter. The outer and inner bandpass filters have no common transmission band, thereby resulting in complete blockage of all optical signals that are not resonantly shifted in wavelength by the intervening atomic vapor. Two embodiments are disclosed, one in which the light signal raises atoms contained in the atomic vapor from the ground state to an excited state from which fluorescence occurs, and the other in which a pump laser is used to raise the atoms in the ground state to a first excited state from which the light signal then is resonantly absorbed, thereby raising the atoms to a second excited state from which fluorescence occurs. A specific application is described in which an optical detector according to the present invention can be used as an underwater detector for light from an optical transmitter which could be located in an orbiting satellite.

Fiber-optic apparatus and method for measurement of luminescence and Raman scattering

DOEpatents

Myrick, M.L.; Angel, S.M.

1993-03-16

A dual fiber forward scattering optrode for Raman spectroscopy with the remote ends of the fibers in opposed, spaced relationship to each other to form a analyte sampling space therebetween and the method of measuring Raman spectra utilizing same are described. One optical fiber is for sending an exciting signal to the remote sampling space and, at its remote end, has a collimating microlens and an optical filter for filtering out background emissions generated in the fiber. The other optical fiber is for collecting the Raman scattering signal at the remote sampling space and, at its remote end, has a collimating microlens and an optical filter to prevent the exciting signal from the exciting fiber from entering the collection fiber and to thereby prevent the generation of background emissions in the collecting fiber.

Time-dependent density functional theory study of the luminescence properties of gold phosphine thiolate complexes.

PubMed

Guidez, Emilie B; Aikens, Christine M

2015-04-09

The origin of the emission of the gold phosphine thiolate complex (TPA)AuSCH(CH3)2 (TPA = 1,3,5-triaza-7-phosphaadamantanetriylphosphine) is investigated using time-dependent density functional theory (TDDFT). This system absorbs light at 3.6 eV, which corresponds mostly to a ligand-to-metal transition with some interligand character. The P-Au-S angle decreases upon relaxation in the S1 and T1 states. Our calculations show that these two states are strongly spin-orbit coupled at the ground state geometry. Ligand effects on the optical properties of this complex are also discussed by looking at the simple AuP(CH3)3SCH3 complex. The excitation energies differ by several tenths of an electronvolt. Excited state optimizations show that the excited singlet and triplet of the (TPA)AuSCH(CH3)2 complex are bent. On the other hand, the Au-S bond breaks in the excited state for the simple complex, and TDDFT is no longer an adequate method. The excited state energy landscape of gold phosphine thiolate systems is very complex, with several state crossings. This study also shows that the formation of the [(TPA)AuSCH(CH3)2]2 dimer is favorable in the ground state. The inclusion of dispersion interactions in the calculations affects the optimized geometries of both ground and excited states. Upon excitation, the formation of a Au-Au bond occurs, which results in an increase in energy of the low energy excited states in comparison to the monomer. The experimentally observed emission of the (TPA)AuSCH(CH3)2 complex at 1.86 eV cannot be unambiguously assigned and may originate from several excited states.

Interband optical pulse injection locking of quantum dot mode-locked semiconductor laser.

PubMed

Kim, Jimyung; Delfyett, Peter J

2008-07-21

We experimentally demonstrate optical clock recovery from quantum dot mode-locked semiconductor lasers by interband optical pulse injection locking. The passively mode-locked slave laser oscillating on the ground state or the first excited state transition is locked through the injection of optical pulses generated via the opposite transition bands, i.e. the first excited state or the ground state transition from the hybridly mode-locked master laser, respectively. When an optical pulse train generated via the first excited state from the master laser is injected to the slave laser oscillating via ground state, the slave laser shows an asymmetric locking bandwidth around the nominal repetition rate of the slave laser. In the reverse injection case of, i.e. the ground state (master laser) to the first excited state (slave laser), the slave laser does not lock even though both lasers oscillate at the same cavity frequency. In this case, the slave laser only locks to higher injection rates as compared to its own nominal repetition rate, and also shows a large locking bandwidth of 6.7 MHz.

Singlet and triplet excitons and charge polarons in cycloparaphenylenes. A density functional theory study

DOE PAGES

Liu, Jin; Adamska, Lyudmyla; Doorn, Stephen K.; ...

2015-05-14

Conformational structure and the electronic properties of various electronic excitations in cycloparaphenylenes (CPPs) are calculated using hybrid Density Functional Theory (DFT). The results demonstrate that wavefunctions of singlet and triplet excitons as well as the positive and negative polarons remain fully delocalized in CPPs. In contrast, these excitations in larger CPP molecules become localized on several phenyl rings, which are locally planarized, while the undeformed ground state geometry is preserved on the rest of the hoop. As evidenced by the measurements of bond-length alternation and dihedral angles, localized regions show stronger hybridization between neighboring bonds and thus enhanced electronic communication.more » This effect is even more significant in the smaller hoops, where phenyl rings have strong quinoid character in the ground state. Thus, upon excitation, electron–phonon coupling leads to the self-trapping of the electronic wavefunction and release of energy from fractions of an eV up to two eVs, depending on the type of excitation and the size of the hoop. The impact of such localization on electronic and optical properties of CPPs is systematically investigated and compared with the available experimental measurements.« less

Relativistic many-body XMCD theory including core degenerate effects

NASA Astrophysics Data System (ADS)

Fujikawa, Takashi

2009-11-01

A many-body relativistic theory to analyze X-ray Magnetic Circular Dichroism (XMCD) spectra has been developed on the basis of relativistic quantum electrodynamic (QED) Keldysh Green's function approach. This theoretical framework enables us to handle relativistic many-body effects in terms of correlated nonrelativistic Green's function and relativistic correction operator Q, which naturally incorporates radiation field screening and other optical field effects in addition to electron-electron interactions. The former can describe the intensity ratio of L2/L3 which deviates from the statistical weight (branching ratio) 1/2. In addition to these effects, we consider the degenerate or nearly degenerate effects of core levels from which photoelectrons are excited. In XPS spectra, for example in Rh 3d sub level excitations, their peak shapes are quite different: This interesting behavior is explained by core-hole moving after the core excitation. We discuss similar problems in X-ray absorption spectra in particular excitation from deep 2p sub levels which are degenerate in each sub levels and nearly degenerate to each other in light elements: The hole left behind is not frozen there. We derive practical multiple scattering formulas which incorporate all those effects.

Effect of the solvent environment on the spectroscopic properties and dynamics of the lowest excited states of carotenoids

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

Frank, H.A.; Bautista, J.A.; Josue, J.

2000-05-11

The spectroscopic properties and dynamics of the lowest excited singlet states of peridinin, fucoxanthin, neoxanthin, uriolide acetate, spheroidene, and spheroidenone in several different solvents have been studied by steady-state absorption and fast-transient optical spectroscopic techniques. Peridinin, fucoxanthin, uriolide acetate, and spheroidenone, which contain carbonyl functional groups in conjugation with the carbon-carbon {pi}-electron system, display broader absorption spectral features and are affected more by the solvent environment than neoxanthin and spheroidene, which do not contain carbonyl functional groups. The possible sources of the spectral broadening are explored by examining the absorption spectra at 77 K in glassy solvents. Also, carotenoids whichmore » contain carbonyls have complex transient absorption spectra and show a pronounced dependence of the excited singlet state lifetime on the solvent environment. It is postulated that these effects are related to the presence of an intramolecular charge transfer state strongly coupled to the S{sub 1} (2{sup 1}A{sub g}) excited singlet state. Structural variations in the series of carotenoids studied here make it possible to focus on the general molecular features that control the spectroscopic and dynamic properties of carotenoids.« less

Small Business Innovations

NASA Technical Reports Server (NTRS)

1996-01-01

Under a Small Business Innovation Research (SBIR) contract to Kennedy Space Center, EIC Laboratories invented a Raman Spectrograph with fiber optic sampling for space applications such as sensing hazardous fuel vapors and making on-board rapid analyses of chemicals and minerals. Raman spectroscopy is a laser-based measurement technique that provides through a unique vibrational spectrum a molecular 'fingerprint,' and can function in aqueous environments. EIC combined optical fiber technology with Raman methods to develop sensors that can be operated at a distance from the spectrographic analysis instruments and the laser excitation source. EIC refined and commercialized the technology to create the Fiber Optic Raman Spectrograph and the RamanProbe. Commercial applications range from process control to monitoring hazardous materials.

Strong Plasmonic Enhancement of a Single Peridinin-Chlorophyll a-Protein Complex on DNA Origami-Based Optical Antennas.

PubMed

Kaminska, Izabela; Bohlen, Johann; Mackowski, Sebastian; Tinnefeld, Philip; Acuna, Guillermo P

2018-02-27

In this contribution, we fabricate hybrid constructs based on a natural light-harvesting complex, peridinin-chlorophyll a-protein, coupled to dimer optical antennas self-assembled with the help of the DNA origami technique. This approach enables controlled positioning of individual complexes at the hotspot of the optical antennas based on large, colloidal gold and silver nanoparticles. Our approach allows us to selectively excite the different pigments present in the harvesting complex, reaching a fluorescence enhancement of 500-fold. This work expands the range of self-assembled functional hybrid constructs for harvesting sunlight and can be further developed for other pigment-proteins and proteins.

Optical Dependence of Electrically Detected Magnetic Resonance in Lightly Doped Si:P Devices

NASA Astrophysics Data System (ADS)

Zhu, Lihuang; van Schooten, Kipp J.; Guy, Mallory L.; Ramanathan, Chandrasekhar

2017-06-01

Using frequency-modulated electrically detected magnetic resonance (EDMR), we show that signals measured from lightly doped (1.2 - 5 ×1 015 cm-3 ) silicon devices vary significantly with the wavelength of the optical excitation used to generate the mobile carriers. We measure EDMR spectra at 4.2 K as a function of modulation frequency and applied microwave power using a 980-nm laser, a 405-nm laser, and a broadband white-light source. EDMR signals are observed from the phosphorus donor and two distinct defect species in all of the experiments. With near-infrared irradiation, we find that the EDMR signal primarily arises from donor-defect pairs, while, at higher photon energies, there are significant additional contributions from defect-defect pairs. The contribution of spins from different spatial regions to the EDMR signal is seen to vary as the optical penetration depth changes from about 120 nm at 405-nm illumination to 100 μ m at 980-nm illumination. The modulation frequency dependence of the EDMR signal shows that the energy of the optical excitation strongly modulates the kinetics of the underlying spin-dependent recombination (SDR) process. Careful tuning of the optical photon energy could therefore be used to control both the subset of spin pairs contributing to the EDMR signal and the dynamics of the SDR process.

Ultra-compact fiber-optic two-photon microscope for functional fluorescence imaging in vivo.

PubMed

Engelbrecht, Christoph J; Johnston, Richard S; Seibel, Eric J; Helmchen, Fritjof

2008-04-14

We present a small, lightweight two-photon fiberscope and demonstrate its suitability for functional imaging in the intact brain. Our device consists of a hollow-core photonic crystal fiber for efficient delivery of near-IR femtosecond laser pulses, a spiral fiber-scanner for resonant beam steering, and a gradient-index lens system for fluorescence excitation, dichroic beam splitting, and signal collection. Fluorescence light is remotely detected using a standard photomultiplier tube. All optical components have 1 mm dimensions and the microscope's headpiece weighs only 0.6 grams. The instrument achieves micrometer resolution at frame rates of typically 25 Hz with a field-of-view of up to 200 microns. We demonstrate functional imaging of calcium signals in Purkinje cell dendrites in the cerebellum of anesthetized rats. The microscope will be easily portable by a rat or mouse and thus should enable functional imaging in freely behaving animals.

Radiation of a resonant medium excited by few-cycle optical pulses at superluminal velocity

NASA Astrophysics Data System (ADS)

Arkhipov, R. M.; Pakhomov, A. V.; Arkhipov, M. V.; Babushkin, I.; Tolmachev, Yu A.; Rosanov, N. N.

2017-05-01

Recent progress in generation of optical pulses of durations comparable to one optical cycle has presented great opportunities for studies of the fundamental processes in matter as well as time-resolved spectroscopy of ultrafast processes in nonlinear media. It opened up a new area of research in modern ultrafast nonlinear optics and led to appearance of the attosecond science. In parallel, a new research area related to emission from resonant media excited by superluminally propagating ultrashort bursts of electromagnetic radiation has been actively developed over the last few years. In this paper, we review our recent results on theoretical analysis of the Cherenkov-type radiation of a resonant medium excited by few-cycle optical pulses propagating at superluminal velocity. This situation can be realized when an electromagnetic pulse with a plane wavefront incidents on a straight string of resonant atoms or a spot of light rotates at very large angular frequency and excites a distant circular string of resonant dipoles. Theoretical analysis revealed some unusual and remarkable features of the Cherenkov radiation generated in this case. This radiation arises in a transient regime which leads to the occurrence of new frequencies in the radiation spectrum. Analysis of the characteristics of this radiation can be used for the study of the resonant structure properties. In addition, a nonlinear resonant medium excited at superluminal velocity can emit unipolar optical pulses, which can be important in ultrafast control of wave-packet dynamics of matter. Specifics of the few-cycle pulse-driven optical response of a resonant medium composed of linear and nonlinear oscillators is discussed.

A density functional theory (DFT) and time-dependent density functional theory (TDDFT) study on optical transitions in oligo(p-phenylenevinylene)-fullerene dyads and the applicability to resonant energy transfer.

PubMed

Toivonen, Teemu L J; Hukka, Terttu I

2007-06-07

The optical transitions of three different size oligo(p-phenylenevinylene)-fullerene dyads (OPV(n)-MPC(60); n = 2-4) and of the corresponding separate molecules are studied using density functional theory (DFT) and time-dependent density functional theory. The DFT is used to determine the geometries and the electronic structures of the ground states. Transition energies and excited-state structures are obtained from the TDDFT calculations. Resonant energy transfer from OPV(n) to MPC(60) is also studied and the Fermi golden rule is used, along with two simple models to describe the electronic coupling to calculate the energy transfer rates. The hybrid-type PBE0 functional is used with a split-valence basis set augmented with a polarization function (SV(P)) in calculations and the calculated results are compared to the corresponding experimental results. The calculated PBE0 spectra of the OPV(n)-MPC(60) dyads correspond to the experimental spectra very well and are approximately sums of the absorption spectra of the separate OPV(n) and MPC(60) molecules. Also, the absorption energies of OPV(n) and MPC(60) and the emission energies of OPV(n) are predicted well with the PBE0 functional. The PBE0 calculated resonant energy transfer rates are in a good agreement with the experimental rates and show the existence of many possible pathways for energy transfer from the first excited singlet states of the OPV(n) molecules to the MPC(60) molecule.

Effect of wetting-layer density of states on the gain and phase recovery dynamics of quantum-dot semiconductor optical amplifiers

NASA Astrophysics Data System (ADS)

Kim, Jungho; Yu, Bong-Ahn

2015-03-01

We numerically investigate the effect of the wetting-layer (WL) density of states on the gain and phase recovery dynamics of quantum-dot semiconductor optical amplifiers in both electrical and optical pumping schemes by solving 1088 coupled rate equations. The temporal variations of the ultrafast gain and phase recovery responses at the ground state (GS) are calculated as a function of the WL density of states. The ultrafast gain recovery responses do not significantly depend on the WL density of states in the electrical pumping scheme and the three optical pumping schemes such as the optical pumping to the WL, the optical pumping to the excited state ensemble, and the optical pumping to the GS ensemble. The ultrafast phase recovery responses are also not significantly affected by the WL density of states except the optical pumping to the WL, where the phase recovery component caused by the WL becomes slowed down as the WL density of states increases.

Fiber-optical switch controlled by a single atom.

PubMed

O'Shea, Danny; Junge, Christian; Volz, Jürgen; Rauschenbeutel, Arno

2013-11-08

We demonstrate highly efficient switching of optical signals between two optical fibers controlled by a single atom. The key element of our experiment is a whispering-gallery-mode bottle microresonator, which is coupled to a single atom and interfaced by two tapered fiber couplers. This system reaches the strong coupling regime of cavity quantum electrodynamics, leading to a vacuum Rabi splitting in the excitation spectrum. We systematically investigate the switching efficiency of our system, i.e., the probability that the fiber-optical switch redirects the light into the desired output. We obtain a large redirection efficiency reaching a raw fidelity of more than 60% without postselection. Moreover, by measuring the second-order correlation functions of the output fields, we show that our switch exhibits a photon-number-dependent routing capability.

Multifocal multiphoton microscopy with adaptive optical correction

NASA Astrophysics Data System (ADS)

Coelho, Simao; Poland, Simon; Krstajic, Nikola; Li, David; Monypenny, James; Walker, Richard; Tyndall, David; Ng, Tony; Henderson, Robert; Ameer-Beg, Simon

2013-02-01

Fluorescence lifetime imaging microscopy (FLIM) is a well established approach for measuring dynamic signalling events inside living cells, including detection of protein-protein interactions. The improvement in optical penetration of infrared light compared with linear excitation due to Rayleigh scattering and low absorption have provided imaging depths of up to 1mm in brain tissue but significant image degradation occurs as samples distort (aberrate) the infrared excitation beam. Multiphoton time-correlated single photon counting (TCSPC) FLIM is a method for obtaining functional, high resolution images of biological structures. In order to achieve good statistical accuracy TCSPC typically requires long acquisition times. We report the development of a multifocal multiphoton microscope (MMM), titled MegaFLI. Beam parallelization performed via a 3D Gerchberg-Saxton (GS) algorithm using a Spatial Light Modulator (SLM), increases TCSPC count rate proportional to the number of beamlets produced. A weighted 3D GS algorithm is employed to improve homogeneity. An added benefit is the implementation of flexible and adaptive optical correction. Adaptive optics performed by means of Zernike polynomials are used to correct for system induced aberrations. Here we present results with significant improvement in throughput obtained using a novel complementary metal-oxide-semiconductor (CMOS) 1024 pixel single-photon avalanche diode (SPAD) array, opening the way to truly high-throughput FLIM.

Tunable emission and excited state absorption induced optical limiting in Tb2(MoO4)3: Sm3+/Eu3+ nanophosphors

NASA Astrophysics Data System (ADS)

Mani, Kamal P.; Sreekanth, Perumbilavil; Vimal, G.; Biju, P. R.; Unnikrishnan, N. V.; Ittyachen, M. A.; Philip, Reji; Joseph, Cyriac

2016-12-01

Photoluminescence properties and optical limiting behavior of pure and Sm3+/Eu3+ doped Tb2(MoO4)3 nanophosphors are investigated. The prepared nanophosphors exhibit excellent emission when excited by UV light. Color-tunable emissions in Tb2-xSmx(MoO4)3 and Tb2-xEux(MoO4)3 are realized by employing different excitation wavelengths or by controlling the doping concentration of Sm3+ and Eu3+. Luminescence quantum yield and CIE chromatic coordinates of the prepared phosphors were also presented. Optical limiting properties of the samples are investigated by open aperture Z-scan technique using 5 ns laser pulses at 532 nm. Numerical fitting of the measured Z-scan data to the relevant nonlinear transmission equations reveals that the nonlinear absorption is arising from strong excited state absorption, along with weak absorption saturation and it is found that the optical nonlinearity of Tb2(MoO4)3 increases with Sm3+/Eu3+doping. Parameters such as saturation fluence, excited state absorption cross section and ground state absorption cross section of the samples have been determined numerically, from which the figure of merit for nonlinear absorption is calculated. The excited state absorption cross-section of the samples is found to be one order of magnitude higher than that of the ground state absorption cross-section, indicating strong reverse saturable absorption. These results indicate that Sm3+/Eu3+ doped Tb2(MoO4)3 nanophosphors are efficient media for UV/n-UV pumped LEDs, and are also potential candidates for designing efficient optical limiting devices for the protection of human eyes and sensitive optical detectors from harmful laser radiation.

Sensitivity enhancement of fluorescence detection in CE by coupling and conducting excitation light with tapered optical fiber.

PubMed

Yang, Xiupei; Huo, Feng; Yuan, Hongyan; Zhang, Bo; Xiao, Dan; Choi, Martin M F

2011-01-01

This paper reports the enhancement of sensitivity of detection for in-column fiber optic-induced fluorescence detection system in CE by tapered optical fiber (TOF). Two types of optical fiber, TOF and conventional cylindrical optical fiber (COF), were employed to construct the CE (TOF-CE and COF-CE) and were compared for sensitivity to riboflavin (RF). The fluorescence intensities from a RF sample with excitation light sources and fibers at various coupling angles were investigated. The fluorescence signal from TOF-CE was ca. ten times that of COF-CE. In addition, the detection performance of four excitation light source-fiber configurations including Laser-TOF, Laser-COF, LED-TOF, and LED-COF were compared. The LODs for RF were 0.21, 0.82, 0.80, and 7.5 nM, respectively, for the four excitation light source-fiber configurations. The results demonstrate that the sensitivity obtained by LED-TOF is close to that of Laser-COF. Both Laser-TOF and LED-TOF can greatly improve the sensitivity of detection in CE. TOF has the major attribute of collecting and focusing the excitation light intensity. Thus, the sensitivity obtained by LED-TOF without focusing lens is just same as that of LED-COF with a focusing lens. This demonstrates that the CE system can be further simplified by eliminating the focusing lens for excitation light. LED-TOF-CE and LED-COF-CE system were applied to the separation and determination of RF in real sample (green tea), respectively. The tapered fiber optic-induced fluorescence detection system in CE is an ideal tool for trace analysis. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

E-MRS Spring Meeting - Nanophotonic Materials Session

DTIC Science & Technology

2004-05-27

are also analyzed, including combinations of recently realized nanorings [5]. The effective optical properties of various families of metamaterials...present calculations of the distant-dependent dissipated power as a function of wave vector for an oscillating dipole above the silver /dielectric...the measurement of leakage radiation to the excitation and propagation of SPPs in silver films with various surface nanostructures, thereby gaining

THz-circuits driven by photo-thermoelectric, gate-tunable graphene-junctions

NASA Astrophysics Data System (ADS)

Brenneis, Andreas; Schade, Felix; Drieschner, Simon; Heimbach, Florian; Karl, Helmut; Garrido, Jose A.; Holleitner, Alexander W.

2016-10-01

For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we exploit ultrafast photo-thermoelectric currents. We describe an immediate photo-thermoelectric current of the unbiased device following a femtosecond laser excitation. For a picosecond time-scale after the optical excitation, an additional photo-thermoelectric contribution shows up, which exhibits the fingerprint of a spatially inverted temperature profile. The latter can be understood by the different time-constants and thermal coupling mechanisms of the electron and phonon baths within graphene to the substrate and the metal contacts. The interplay of the processes gives rise to ultrafast electromagnetic transients in high-frequency circuits, and it is equally important for a fundamental understanding of graphene-based ultrafast photodetectors and switches.

THz-circuits driven by photo-thermoelectric, gate-tunable graphene-junctions

PubMed Central

Brenneis, Andreas; Schade, Felix; Drieschner, Simon; Heimbach, Florian; Karl, Helmut; Garrido, Jose A.; Holleitner, Alexander W.

2016-01-01

For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we exploit ultrafast photo-thermoelectric currents. We describe an immediate photo-thermoelectric current of the unbiased device following a femtosecond laser excitation. For a picosecond time-scale after the optical excitation, an additional photo-thermoelectric contribution shows up, which exhibits the fingerprint of a spatially inverted temperature profile. The latter can be understood by the different time-constants and thermal coupling mechanisms of the electron and phonon baths within graphene to the substrate and the metal contacts. The interplay of the processes gives rise to ultrafast electromagnetic transients in high-frequency circuits, and it is equally important for a fundamental understanding of graphene-based ultrafast photodetectors and switches. PMID:27762291

THz-circuits driven by photo-thermoelectric, gate-tunable graphene-junctions.

PubMed

Brenneis, Andreas; Schade, Felix; Drieschner, Simon; Heimbach, Florian; Karl, Helmut; Garrido, Jose A; Holleitner, Alexander W

2016-10-20

For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we exploit ultrafast photo-thermoelectric currents. We describe an immediate photo-thermoelectric current of the unbiased device following a femtosecond laser excitation. For a picosecond time-scale after the optical excitation, an additional photo-thermoelectric contribution shows up, which exhibits the fingerprint of a spatially inverted temperature profile. The latter can be understood by the different time-constants and thermal coupling mechanisms of the electron and phonon baths within graphene to the substrate and the metal contacts. The interplay of the processes gives rise to ultrafast electromagnetic transients in high-frequency circuits, and it is equally important for a fundamental understanding of graphene-based ultrafast photodetectors and switches.

Optical patterning of trapped charge in nitrogen-doped diamond

NASA Astrophysics Data System (ADS)

Jayakumar, Harishankar; Henshaw, Jacob; Dhomkar, Siddharth; Pagliero, Daniela; Laraoui, Abdelghani; Manson, Neil B.; Albu, Remus; Doherty, Marcus W.; Meriles, Carlos A.

2016-08-01

The nitrogen-vacancy (NV) centre in diamond is emerging as a promising platform for solid-state quantum information processing and nanoscale metrology. Of interest in these applications is the manipulation of the NV charge, which can be attained by optical excitation. Here, we use two-colour optical microscopy to investigate the dynamics of NV photo-ionization, charge diffusion and trapping in type-1b diamond. We combine fixed-point laser excitation and scanning fluorescence imaging to locally alter the concentration of negatively charged NVs, and to subsequently probe the corresponding redistribution of charge. We uncover the formation of spatial patterns of trapped charge, which we qualitatively reproduce via a model of the interplay between photo-excited carriers and atomic defects. Further, by using the NV as a probe, we map the relative fraction of positively charged nitrogen on localized optical excitation. These observations may prove important to transporting quantum information between NVs or to developing three-dimensional, charge-based memories.

Optical oscillator strengths of the valence-shell excitations of atoms and molecules determined by the dipole ( γ,γ) method

NASA Astrophysics Data System (ADS)

Xu, Long-Quan; Liu, Ya-Wei; Xu, Xin; Ni, Dong-Dong; Yang, Ke; Zhu, Lin-Fan

2017-07-01

The dipole (γ,γ) method, which is the inelastic X-ray scattering operated at a negligibly small momentum transfer, has been developed to determine the absolute optical oscillator strengths of the valence-shell excitations of atoms and molecules. This new method is free from the line saturation effect, and its Bethe-Born conversion factor varies much more slowly with the excitation energy than that of the dipole (e, e) method. Thus the dipole (γ,γ) method provides a reliable approach to obtain the benchmark optical oscillator strengths of the valence-shell excitations for gaseous atoms and molecules. In this paper, we give a review of the dipole (γ,γ) method and some recent measurements of absolute optical oscillator strengths of gaseous atoms and molecules. Contribution to the Topical Issue "Atomic and Molecular Data and their Applications", edited by Gordon W.F. Drake, Jung-Sik Yoon, Daiji Kato, Grzegorz Karwasz.

Optical patterning of trapped charge in nitrogen-doped diamond.

PubMed

Jayakumar, Harishankar; Henshaw, Jacob; Dhomkar, Siddharth; Pagliero, Daniela; Laraoui, Abdelghani; Manson, Neil B; Albu, Remus; Doherty, Marcus W; Meriles, Carlos A

2016-08-30

The nitrogen-vacancy (NV) centre in diamond is emerging as a promising platform for solid-state quantum information processing and nanoscale metrology. Of interest in these applications is the manipulation of the NV charge, which can be attained by optical excitation. Here, we use two-colour optical microscopy to investigate the dynamics of NV photo-ionization, charge diffusion and trapping in type-1b diamond. We combine fixed-point laser excitation and scanning fluorescence imaging to locally alter the concentration of negatively charged NVs, and to subsequently probe the corresponding redistribution of charge. We uncover the formation of spatial patterns of trapped charge, which we qualitatively reproduce via a model of the interplay between photo-excited carriers and atomic defects. Further, by using the NV as a probe, we map the relative fraction of positively charged nitrogen on localized optical excitation. These observations may prove important to transporting quantum information between NVs or to developing three-dimensional, charge-based memories.

Optical patterning of trapped charge in nitrogen-doped diamond

PubMed Central

Jayakumar, Harishankar; Henshaw, Jacob; Dhomkar, Siddharth; Pagliero, Daniela; Laraoui, Abdelghani; Manson, Neil B.; Albu, Remus; Doherty, Marcus W.; Meriles, Carlos A.

2016-01-01

The nitrogen-vacancy (NV) centre in diamond is emerging as a promising platform for solid-state quantum information processing and nanoscale metrology. Of interest in these applications is the manipulation of the NV charge, which can be attained by optical excitation. Here, we use two-colour optical microscopy to investigate the dynamics of NV photo-ionization, charge diffusion and trapping in type-1b diamond. We combine fixed-point laser excitation and scanning fluorescence imaging to locally alter the concentration of negatively charged NVs, and to subsequently probe the corresponding redistribution of charge. We uncover the formation of spatial patterns of trapped charge, which we qualitatively reproduce via a model of the interplay between photo-excited carriers and atomic defects. Further, by using the NV as a probe, we map the relative fraction of positively charged nitrogen on localized optical excitation. These observations may prove important to transporting quantum information between NVs or to developing three-dimensional, charge-based memories. PMID:27573190

Bosonic excitations and electron pairing in an electron-doped cuprate superconductor

NASA Astrophysics Data System (ADS)

Wang, M. C.; Yu, H. S.; Xiong, J.; Yang, Y.-F.; Luo, S. N.; Jin, K.; Qi, J.

2018-04-01

By applying ultrafast optical spectroscopy to electron-doped La1.9Ce0.1CuO4 ±δ , we discern a bosonic mode of electronic origin and provide the evolution of its coupling with the charge carriers as a function of temperature. Our results show that it has the strongest coupling strength near Tc and can fully account for the superconducting pairing. This mode can be associated with the two-dimensional antiferromagnetic spin correlations emerging below a critical temperature T† larger than Tc. Our work may help to establish a quantitative relation between bosonic excitations and superconducting pairing in electron-doped cuprates.

Subcycle dynamics of high-order-harmonic generation of He atoms excited by attosecond pulses and driven by near-infrared laser fields: A self-interaction-free time-dependent density-functional-theory approach

NASA Astrophysics Data System (ADS)

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

2014-05-01

In the framework of the self-interaction-free time-dependent density-functional theory, we have performed three-dimensional (3D) ab initio calculations of He atoms in near-infrared (NIR) laser fields subject to excitation by a single extreme ultraviolet (XUV) attosecond pulse (SAP). We have explored the dynamical behavior of the subcycle high harmonic generation (HHG) for transitions from the excited states to the ground state and found oscillation structures with respect to the time delay between the SAP and NIR fields. The oscillatory pattern in the photon emission spectra has a period of ˜1.3 fs which is half of the NIR laser optical cycle, similar to that recently measured in the experiments on transient absorption of He [M. Chini et al., Sci. Rep. 3, 1105 (2013), 10.1038/srep01105]. We present the photon emission spectra from 1s2p, 1s3p, 1s4p, 1s5p, and 1s6p excited states as functions of the time delay. We explore the subcycle Stark shift phenomenon in NIR fields and its influence on the photon emission process. Our analysis reveals several interesting features of the subcycle HHG dynamics and we identify the mechanisms responsible for the observed peak splitting in the photon emission spectra.

A rapid excitation-emission matrix fluorometer utilizing supercontinuum white light and acousto-optic tunable filters

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

Wang, Wenbo; Department of Dermatology and Skin Science, University of British Columbia, 835 West 10th Avenue, Vancouver, British Columbia V5Z 4E8; Department of Biomedical Engineering, University of British Columbia, KAIS 5500, 2332 Main Mall, Vancouver, British Columbia V6T 1Z4

Scanning speed and coupling efficiency of excitation light to optic fibres are two major technical challenges that limit the potential of fluorescence excitation-emission matrix (EEM) spectrometer for on-line applications and in vivo studies. In this paper, a novel EEM system, utilizing a supercontinuum white light source and acousto-optic tunable filters (AOTFs), was introduced and evaluated. The supercontinuum white light, generated by pumping a nonlinear photonic crystal fiber with an 800 nm femtosecond laser, was efficiently coupled into a bifurcated optic fiber bundle. High speed EEM spectral scanning was achieved using AOTFs both for selecting excitation wavelength and scanning emission spectra.more » Using calibration lamps (neon and mercury argon), wavelength deviations were determined to vary from 0.18 nm to −0.70 nm within the spectral range of 500–850 nm. Spectral bandwidth for filtered excitation light broadened by twofold compared to that measured with monochromatic light between 650 nm and 750 nm. The EEM spectra for methanol solutions of laser dyes were successfully acquired with this rapid fluorometer using an integration time of 5 s.« less

Time-domain measurement of optical transport in silicon micro-ring resonators.

PubMed

Pernice, Wolfram H P; Li, Mo; Tang, Hong X

2010-08-16

We perform time-domain measurements of optical transport dynamics in silicon nano-photonic devices. Using pulsed optical excitation the thermal and carrier induced optical nonlinearities of micro-ring resonators are investigated, allowing for identification of their individual contributions. Under pulsed excitation build-up of free carriers and heat in the waveguides leads to a beating oscillation of the cavity resonance frequency. When employing a burst of pulse trains shorter than the carrier life-time, the slower heating effect can be separated from the faster carrier effect. Our scheme provides a convenient way to thermally stabilize optical resonators for high-power time-domain applications and nonlinear optical conversion.

Charge-transfer optical absorption mechanism of DNA:Ag-nanocluster complexes

NASA Astrophysics Data System (ADS)

Longuinhos, R.; Lúcio, A. D.; Chacham, H.; Alexandre, S. S.

2016-05-01

Optical properties of DNA:Ag-nanoclusters complexes have been successfully applied experimentally in Chemistry, Physics, and Biology. Nevertheless, the mechanisms behind their optical activity remain unresolved. In this work, we present a time-dependent density functional study of optical absorption in DNA:Ag4. In all 23 different complexes investigated, we obtain new absorption peaks in the visible region that are not found in either the isolated Ag4 or isolated DNA base pairs. Absorption from red to green are predominantly of charge-transfer character, from the Ag4 to the DNA fragment, while absorption in the blue-violet range are mostly associated to electronic transitions of a mixed character, involving either DNA-Ag4 hybrid orbitals or intracluster orbitals. We also investigate the role of exchange-correlation functionals in the calculated optical spectra. Significant differences are observed between the calculations using the PBE functional (without exact exchange) and the CAM-B3LYP functional (which partly includes exact exchange). Specifically, we observe a tendency of charge-transfer excitations to involve purines bases, and the PBE spectra error is more pronounced in the complexes where the Ag cluster is bound to the purines. Finally, our results also highlight the importance of adding both the complementary base pair and the sugar-phosphate backbone in order to properly characterize the absorption spectrum of DNA:Ag complexes.

Charge-transfer optical absorption mechanism of DNA:Ag-nanocluster complexes.

PubMed

Longuinhos, R; Lúcio, A D; Chacham, H; Alexandre, S S

2016-05-01

Optical properties of DNA:Ag-nanoclusters complexes have been successfully applied experimentally in Chemistry, Physics, and Biology. Nevertheless, the mechanisms behind their optical activity remain unresolved. In this work, we present a time-dependent density functional study of optical absorption in DNA:Ag_{4}. In all 23 different complexes investigated, we obtain new absorption peaks in the visible region that are not found in either the isolated Ag_{4} or isolated DNA base pairs. Absorption from red to green are predominantly of charge-transfer character, from the Ag_{4} to the DNA fragment, while absorption in the blue-violet range are mostly associated to electronic transitions of a mixed character, involving either DNA-Ag_{4} hybrid orbitals or intracluster orbitals. We also investigate the role of exchange-correlation functionals in the calculated optical spectra. Significant differences are observed between the calculations using the PBE functional (without exact exchange) and the CAM-B3LYP functional (which partly includes exact exchange). Specifically, we observe a tendency of charge-transfer excitations to involve purines bases, and the PBE spectra error is more pronounced in the complexes where the Ag cluster is bound to the purines. Finally, our results also highlight the importance of adding both the complementary base pair and the sugar-phosphate backbone in order to properly characterize the absorption spectrum of DNA:Ag complexes.

Observation of sub-100-fs optical response from spin-coated films of squarylium dye J aggregates

NASA Astrophysics Data System (ADS)

Furuki, Makoto; Tian, Minquan; Sato, Yasuhiro; Pu, Lyong Sun; Kawashima, Hitoshi; Tatsuura, Satoshi; Wada, Osamu

2001-04-01

For spin-coated films of squarylium dye J aggregates, ultrafast nonlinear optical responses were investigated by pump-probe measurements. By using a broadband mode-locked titanium:sapphire laser, we succeeded in observing the optical response with a time resolution of better than 60 fs. Time-resolved transmission data are shown for different excitation wavelengths, resonant to the excitonic absorption band and off-resonant. Relaxation times of the absorption saturation were evaluated to be 140 fs (fast component) and 950 fs (slow component) in the case of resonant excitation and 98 fs in the case of off-resonant excitation.

Intermolecular electron transfer from intramolecular excitation and coherent acoustic phonon generation in a hydrogen-bonded charge-transfer solid

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

Rury, Aaron S., E-mail: arury@usc.edu; Sorenson, Shayne; Dawlaty, Jahan M.

2016-03-14

Organic materials that produce coherent lattice phonon excitations in response to external stimuli may provide next generation solutions in a wide range of applications. However, for these materials to lead to functional devices in technology, a full understanding of the possible driving forces of coherent lattice phonon generation must be attained. To facilitate the achievement of this goal, we have undertaken an optical spectroscopic study of an organic charge-transfer material formed from the ubiquitous reduction-oxidation pair hydroquinone and p-benzoquinone. Upon pumping this material, known as quinhydrone, on its intermolecular charge transfer resonance as well as an intramolecular resonance of p-benzoquinone,more » we find sub-cm{sup −1} oscillations whose dispersion with probe energy resembles that of a coherent acoustic phonon that we argue is coherently excited following changes in the electron density of quinhydrone. Using the dynamical information from these ultrafast pump-probe measurements, we find that the fastest process we can resolve does not change whether we pump quinhydrone at either energy. Electron-phonon coupling from both ultrafast coherent vibrational and steady-state resonance Raman spectroscopies allows us to determine that intramolecular electronic excitation of p-benzoquinone also drives the electron transfer process in quinhydrone. These results demonstrate the wide range of electronic excitations of the parent of molecules found in many functional organic materials that can drive coherent lattice phonon excitations useful for applications in electronics, photonics, and information technology.« less

Intermolecular electron transfer from intramolecular excitation and coherent acoustic phonon generation in a hydrogen-bonded charge-transfer solid

NASA Astrophysics Data System (ADS)

Rury, Aaron S.; Sorenson, Shayne; Dawlaty, Jahan M.

2016-03-01

Organic materials that produce coherent lattice phonon excitations in response to external stimuli may provide next generation solutions in a wide range of applications. However, for these materials to lead to functional devices in technology, a full understanding of the possible driving forces of coherent lattice phonon generation must be attained. To facilitate the achievement of this goal, we have undertaken an optical spectroscopic study of an organic charge-transfer material formed from the ubiquitous reduction-oxidation pair hydroquinone and p-benzoquinone. Upon pumping this material, known as quinhydrone, on its intermolecular charge transfer resonance as well as an intramolecular resonance of p-benzoquinone, we find sub-cm-1 oscillations whose dispersion with probe energy resembles that of a coherent acoustic phonon that we argue is coherently excited following changes in the electron density of quinhydrone. Using the dynamical information from these ultrafast pump-probe measurements, we find that the fastest process we can resolve does not change whether we pump quinhydrone at either energy. Electron-phonon coupling from both ultrafast coherent vibrational and steady-state resonance Raman spectroscopies allows us to determine that intramolecular electronic excitation of p-benzoquinone also drives the electron transfer process in quinhydrone. These results demonstrate the wide range of electronic excitations of the parent of molecules found in many functional organic materials that can drive coherent lattice phonon excitations useful for applications in electronics, photonics, and information technology.

sp-d Exchange Interactions in Wave Function Engineered Colloidal CdSe/Mn:CdS Hetero-Nanoplatelets.

PubMed

Muckel, Franziska; Delikanli, Savas; Hernández-Martínez, Pedro Ludwig; Priesner, Tamara; Lorenz, Severin; Ackermann, Julia; Sharma, Manoj; Demir, Hilmi Volkan; Bacher, Gerd

2018-03-14

In two-dimensional (2D) colloidal semiconductor nanoplatelets, which are atomically flat nanocrystals, the precise control of thickness and composition on the atomic scale allows for the synthesis of heterostructures with well-defined electron and hole wave function distributions. Introducing transition metal dopants with a monolayer precision enables tailored magnetic exchange interactions between dopants and band states. Here, we use the absorption based technique of magnetic circular dichroism (MCD) to directly prove the exchange coupling of magnetic dopants with the band charge carriers in hetero-nanoplatelets with CdSe core and manganese-doped CdS shell (CdSe/Mn:CdS). We show that the strength of both the electron as well as the hole exchange interactions with the dopants can be tuned by varying the nanoplatelets architecture with monolayer accuracy. As MCD is highly sensitive for excitonic resonances, excited level spectroscopy allows us to resolve and identify, in combination with wave function calculations, several excited state transitions including spin-orbit split-off excitonic contributions. Thus, our study not only demonstrates the possibility to expand the extraordinary physical properties of colloidal nanoplatelets toward magneto-optical functionality by transition metal doping but also provides an insight into the excited state electronic structure in this novel two-dimensional material.

Stimulated Raman photoacoustic imaging

PubMed Central

Yakovlev, Vladislav V.; Zhang, Hao F.; Noojin, Gary D.; Denton, Michael L.; Thomas, Robert J.; Scully, Marlan O.

2010-01-01

Achieving label-free, molecular-specific imaging with high spatial resolution in deep tissue is often considered the grand challenge of optical imaging. To accomplish this goal, significant optical scattering in tissues has to be overcome while achieving molecular specificity without resorting to extrinsic labeling. We demonstrate the feasibility of developing such an optical imaging modality by combining the molecularly specific stimulated Raman excitation with the photoacoustic detection. By employing two ultrashort excitation laser pulses, separated in frequency by the vibrational frequency of a targeted molecule, only the specific vibrational level of the target molecules in the illuminated tissue volume is excited. This targeted optical absorption generates ultrasonic waves (referred to as stimulated Raman photoacoustic waves) which are detected using a traditional ultrasonic transducer to form an image following the design of the established photoacoustic microscopy. PMID:21059930

Dopant concentration dependent optical and X-Ray induced photoluminescence in Eu3+ doped La2Zr2O7

NASA Astrophysics Data System (ADS)

Pokhrel, Madhab; Brik, Mikhail; Mao, Yuanbing

2015-03-01

Herein, we will be presenting the dopant (Eu) concentration dependent high density La2Zr2O7 nanoparticles for optical and X-ray scintillation applications by use of X - ray diffraction, Raman, FTIR, scanning electron microscope (SEM), transmission electron microscopy (TEM), optically and X-ray excited photoluminescence (PL). Several theoretical methods have been used in order to investigate the structural, electronic, optical, elastic, dynamic properties of Eu doped La2Zr2O7. It is observed that Eu: La2Zr2O7 shows an intense red luminescence under 258, 322, 394 and 465 nm excitation. The optical intensity of Eu: La2Zr2O7 depends on the dopant concentration of Eu3+. Following high energy excitation with X-rays, Eu: La2Zr2O7 shows an atypical Eu PL response (scintillation) with a red emission. The intense color emission of Eu obtained under 258 nm excitation, the X-ray induced luminescence property along with reportedly high density of La2Zr2O7, makes these nanomaterials attractive for optical and X-ray applications. The authors thank the support from the Defense Threat Reduction Agency (DTRA) of the U.S. Department of Defense (Award #HDTRA1-10-1-0114).

Harnessing molecular excited states with Lanczos chains.

PubMed

Baroni, Stefano; Gebauer, Ralph; Bariş Malcioğlu, O; Saad, Yousef; Umari, Paolo; Xian, Jiawei

2010-02-24

The recursion method of Haydock, Heine and Kelly is a powerful tool for calculating diagonal matrix elements of the resolvent of quantum-mechanical Hamiltonian operators by elegantly expressing them in terms of continued fractions. In this paper we extend the recursion method to off-diagonal matrix elements of general (possibly non-Hermitian) operators and apply it to the simulation of molecular optical absorption and photoemission spectra within time-dependent density-functional and many-body perturbation theories, respectively. This method is demonstrated with a couple of applications to the optical absorption and photoemission spectra of the caffeine molecule.

Multi-function diamond film fiberoptic probe and measuring system employing same

DOEpatents

Young, Jack P.

1998-01-01

A fused fiberoptic probe having a protective cover, a fiberoptic probe system, and embodiments thereof for conducting electromagnetic spectral measurements are disclosed. The fused fiberoptic probe comprises a probe tip having a specific geometrical configuration, an exciting optical fiber and at least one collection optical fiber fused within a housing, preferrably silica, with a protective cover disposed over at least a portion of the probe tip. The specific geometrical configurations in which the probe tip can be shaped include a slanted probe tip with an angle greater than 0.degree., an inverted cone-shaped probe tip, and a lens head.

Harnessing molecular excited states with Lanczos chains

NASA Astrophysics Data System (ADS)

Baroni, Stefano; Gebauer, Ralph; Bariş Malcioğlu, O.; Saad, Yousef; Umari, Paolo; Xian, Jiawei

2010-02-01

The recursion method of Haydock, Heine and Kelly is a powerful tool for calculating diagonal matrix elements of the resolvent of quantum-mechanical Hamiltonian operators by elegantly expressing them in terms of continued fractions. In this paper we extend the recursion method to off-diagonal matrix elements of general (possibly non-Hermitian) operators and apply it to the simulation of molecular optical absorption and photoemission spectra within time-dependent density-functional and many-body perturbation theories, respectively. This method is demonstrated with a couple of applications to the optical absorption and photoemission spectra of the caffeine molecule.

Exciton scattering approach for optical spectra calculations in branched conjugated macromolecules

NASA Astrophysics Data System (ADS)

Li, Hao; Wu, Chao; Malinin, Sergey V.; Tretiak, Sergei; Chernyak, Vladimir Y.

2016-12-01

The exciton scattering (ES) technique is a multiscale approach based on the concept of a particle in a box and developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, electronic excitations in molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph whose edges and nodes stand for the molecular linear segments and vertices, respectively. Exciton propagation on the linear segments is characterized by the exciton dispersion, whereas exciton scattering at the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized "particle in a box" problems on the graph that represents the molecule. Similarly, unique energy-dependent ES dipolar parameters permit calculations of the corresponding oscillator strengths, thus, completing optical spectra modeling. Both the energetic and dipolar parameters can be extracted from quantum-chemical computations in small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within a considered molecular family could be performed with negligible numerical effort. We demonstrate the ES method application to molecular families of branched conjugated phenylacetylenes and ladder poly-para-phenylenes, as well as structures with electron donor and acceptor chemical substituents. Time-dependent density functional theory (TD-DFT) is used as a reference model for electronic structure. The ES calculations accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

Non-resonant excitation of rare-earth ions via virtual Auger process

NASA Astrophysics Data System (ADS)

Yassievich, I. N.

2011-05-01

The luminescence of rare-earth ions (REI) is often intensified by defects associated with REIs or excitons bound to these defects. In this paper we show that the presence of such a state opens the possibility of non-resonance optical pumping via the process involving virtual Auger transition. It is the second order perturbation process when an electron arrives in an virtual intermediate state due to the optical transition (the first step) and the Auger transition is the second one. We have calculated the cross-section of such an excitation process when the optical transition is accompanied by creation of the exciton bound to the defect associated with REI and obtained a simple analytical expression for the cross-section. The excess energy of the excitation quanta is taken away by multiphonon emission. The electron-phonon interaction with local phonon vibrations of the bound exciton is assumed to determine the multiphonon process. It is shown that the probability of the process under study exceeds considerably the probability of direct optical 4f-4f absorption even in the case when the energy distance between the excitation quantum energy and the exciton energy is about 0.1 of the exciton energy. The excitation mechanism considered leads to the appearance of a broad unsymmetrical band in the excitation spectrum with the red side much wider and flatter than the blue one.

Berkeley Lab - Materials Sciences Division

Science.gov Websites

Computational Study of Excited-State Phenomena in Energy Materials Center for X-ray Optics MSD Facilities Ion Excited-State Phenomena in Energy Materials Center for X-ray Optics MSD Facilities Ion Beam Analysis Behavior of Lithium Metal across a Rigid Block Copolymer Electrolyte Membrane. Journal of the

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.

Investigation of in-flame soot optical properties in laminar coflow diffusion flames using thermophoretic particle sampling and spectral light extinction

NASA Astrophysics Data System (ADS)

Kempema, Nathan J.; Ma, Bin; Long, Marshall B.

2016-09-01

Soot optical properties are essential to the noninvasive study of the in-flame evolution of soot particles since they allow quantitative interpretation of optical diagnostics. Such experimental data are critical for comparison to results from computational models and soot sub-models. In this study, the thermophoretic sampling particle diagnostic (TSPD) technique is applied along with data from a previous spectrally resolved line-of-sight light attenuation experiment to determine the soot volume fraction and absorption function. The TSPD technique is applied in a flame stabilized on the Yale burner, and the soot scattering-to-absorption ratio is calculated using the Rayleigh-Debye-Gans theory for fractal aggregates and morphology information from a previous sampling experiment. The soot absorption function is determined as a function of wavelength and found to be in excellent agreement with previous in-flame measurements of the soot absorption function in coflow laminar diffusion flames. Two-dimensional maps of the soot dispersion exponent are calculated and show that the soot absorption function may have a positive or negative exponential wavelength dependence depending on the in-flame location. Finally, the wavelength dependence of the soot absorption function is related to the ratio of soot absorption functions, as would be found using two-excitation-wavelength laser-induced incandescence.

Multiscale modeling and computation of optically manipulated nano devices

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

Bao, Gang, E-mail: baog@zju.edu.cn; Liu, Di, E-mail: richardl@math.msu.edu; Luo, Songting, E-mail: luos@iastate.edu

2016-07-01

We present a multiscale modeling and computational scheme for optical-mechanical responses of nanostructures. The multi-physical nature of the problem is a result of the interaction between the electromagnetic (EM) field, the molecular motion, and the electronic excitation. To balance accuracy and complexity, we adopt the semi-classical approach that the EM field is described classically by the Maxwell equations, and the charged particles follow the Schrödinger equations quantum mechanically. To overcome the numerical challenge of solving the high dimensional multi-component many-body Schrödinger equations, we further simplify the model with the Ehrenfest molecular dynamics to determine the motion of the nuclei, andmore » use the Time-Dependent Current Density Functional Theory (TD-CDFT) to calculate the excitation of the electrons. This leads to a system of coupled equations that computes the electromagnetic field, the nuclear positions, and the electronic current and charge densities simultaneously. In the regime of linear responses, the resonant frequencies initiating the out-of-equilibrium optical-mechanical responses can be formulated as an eigenvalue problem. A self-consistent multiscale method is designed to deal with the well separated space scales. The isomerization of azobenzene is presented as a numerical example.« less

Optically programmable encoder based on light propagation in two-dimensional regular nanoplates.

PubMed

Li, Ya; Zhao, Fangyin; Guo, Shuai; Zhang, Yongyou; Niu, Chunhui; Zeng, Ruosheng; Zou, Bingsuo; Zhang, Wensheng; Ding, Kang; Bukhtiar, Arfan; Liu, Ruibin

2017-04-07

We design an efficient optically controlled microdevice based on CdSe nanoplates. Two-dimensional CdSe nanoplates exhibit lighting patterns around the edges and can be realized as a new type of optically controlled programmable encoder. The light source is used to excite the nanoplates and control the logical position under vertical pumping mode by the objective lens. At each excitation point in the nanoplates, the preferred light-propagation routes are along the normal direction and perpendicular to the edges, which then emit out from the edges to form a localized lighting section. The intensity distribution around the edges of different nanoplates demonstrates that the lighting part with a small scale is much stronger, defined as '1', than the dark section, defined as '0', along the edge. These '0' and '1' are the basic logic elements needed to compose logically functional devices. The observed propagation rules are consistent with theoretical simulations, meaning that the guided-light route in two-dimensional semiconductor nanoplates is regular and predictable. The same situation was also observed in regular CdS nanoplates. Basic theoretical analysis and experiments prove that the guided light and exit position follow rules mainly originating from the shape rather than material itself.

Effect of the band structure in a rigorous two-body model with long-range interactions in 1D optical lattices

NASA Astrophysics Data System (ADS)

Kristensen, Tom; Simoni, Andrea; Launay, Jean-Michel

2016-05-01

We compute scattering and bound state properties for two ultracold molecules in a pure 1D optical lattice. We introduce reference functions with complex quasi-momentum that naturally account for the effect of excited energy bands. Our exact results for a short-range interaction are first compared with the simplest version of the standard Bose-Hubbard (BH) model. Such comparison allows us to highlight the effect of the excited bands, of the non-on-site interaction and of tunneling with distant neighbor, that are not taken into account in the BH model. The effective interaction can depend strongly on the particle quasi-momenta and can present a resonant behavior even in a deep lattice. As a second step, we study scattering of two polar particles in the optical lattice. Peculiar Wigner threshold laws stem from the interplay of the long range dipolar interaction and the presence of the energy bands. We finally assess the validity of an extended Bose-Hubbard model for dipolar gases based on our exact two-body calculations. This work was supported by the Agence Nationale de la Recherche (Contract No. ANR-12-BS04-0020-01).

Optical element for full spectral purity from IR-generated EUV light sources

NASA Astrophysics Data System (ADS)

van den Boogaard, A. J. R.; Louis, E.; van Goor, F. A.; Bijkerk, F.

2009-03-01

Laser produced plasma (LLP) sources are generally considered attractive for high power EUV production in next generation lithography equipment. Such plasmas are most efficiently excited by the relatively long, infrared wavelengths of CO2-lasers, but a significant part of the rotational-vibrational excitation lines of the CO2 radiation will be backscattered by the plasma's critical density surface and consequently will be present as parasitic radiation in the spectrum of such sources. Since most optical elements in the EUV collecting and imaging train have a high reflection coefficient for IR radiation, undesirable heating phenomena at the resist level are likely to occur. In this study a completely new principle is employed to obtain full separation of EUV and IR radiation from the source by a single optical component. While the application of a transmission filter would come at the expense of EUV throughput, this technique potentially enables wavelength separation without loosing reflectance compared to a conventional Mo/Si multilayer coated element. As a result this method provides full spectral purity from the source without loss in EUV throughput. Detailed calculations on the principal of functioning are presented.

Enhanced antibody recognition with a magneto-optic surface plasmon resonance (MO-SPR) sensor.

PubMed

Manera, Maria Grazia; Ferreiro-Vila, Elías; Garcia-Martin, José Miguel; Garcia-Martin, Antonio; Rella, Roberto

2014-08-15

A comparison between sensing performance of traditional SPR (Surface Plasmon Resonance) and magneto-optic SPR (MOSPR) transducing techniques is presented in this work. MOSPR comes from an evolution of traditional SPR platform aiming at modulating Surface Plasmon wave by the application of an external magnetic field in transverse configuration. Previous work demonstrated that, when the Plasmon resonance is excited in these structures, the external magnetic field induces a modification of the coupling of the incident light with the Surface Plasmon Polaritons (SPP). Besides, these structures can lead to an enhancement in the magneto-optical (MO) activity when the SPP is excited. This phenomenon is exploited in this work to demonstrate the possibility to use the enhanced MO signal as proper transducer signal for investigating biomolecular interactions in liquid phase. To this purpose, the transducer surface was functionalized by thiol chemistry and used for recording the binding between Bovine Serum Albumin molecules immobilized onto the surface and its complementary target. Higher sensing performance in terms of sensitivity and lower limit of detection of the MOSPR biosensor with respect to traditional SPR sensors is demonstrated. Copyright © 2014 Elsevier B.V. All rights reserved.

Laser Pulse Duration Is Critical For the Generation of Plasmonic Nanobubbles

PubMed Central

2015-01-01

Plasmonic nanobubbles (PNBs) are transient vapor nanobubbles generated in liquid around laser-overheated plasmonic nanoparticles. Unlike plasmonic nanoparticles, PNBs’ properties are still largely unknown due to their highly nonstationary nature. Here we show the influence of the duration of the optical excitation on the energy efficacy and threshold of PNB generation. The combination of picosecond pulsed excitation with the nanoparticle clustering provides the highest energy efficacy and the lowest threshold fluence, around 5 mJ cm–2, of PNB generation. In contrast, long excitation pulses reduce the energy efficacy of PNB generation by several orders of magnitude. Ultimately, the continuous excitation has the minimal energy efficacy, nine orders of magnitude lower than that for the picosecond excitation. Thus, the duration of the optical excitation of plasmonic nanoparticles can have a stronger effect on the PNB generation than the excitation wavelength, nanoparticle size, shape, or other “stationary” properties of plasmonic nanoparticles. PMID:24916057

Time-resolved x-ray absorption spectroscopy: Watching atoms dance

NASA Astrophysics Data System (ADS)

Milne, Chris J.; Pham, Van-Thai; Gawelda, Wojciech; van der Veen, Renske M.; El Nahhas, Amal; Johnson, Steven L.; Beaud, Paul; Ingold, Gerhard; Lima, Frederico; Vithanage, Dimali A.; Benfatto, Maurizio; Grolimund, Daniel; Borca, Camelia; Kaiser, Maik; Hauser, Andreas; Abela, Rafael; Bressler, Christian; Chergui, Majed

2009-11-01

The introduction of pump-probe techniques to the field of x-ray absorption spectroscopy (XAS) has allowed the monitoring of both structural and electronic dynamics of disordered systems in the condensed phase with unprecedented accuracy, both in time and in space. We present results on the electronically excited high-spin state structure of an Fe(II) molecular species, [FeII(bpy)3]2+, in aqueous solution, resolving the Fe-N bond distance elongation as 0.2 Å. In addition an analysis technique using the reduced χ2 goodness of fit between FEFF EXAFS simulations and the experimental transient absorption signal in energy space has been successfully tested as a function of excited state population and chemical shift, demonstrating its applicability in situations where the fractional excited state population cannot be determined through other measurements. Finally by using a novel ultrafast hard x-ray 'slicing' source the question of how the molecule relaxes after optical excitation has been successfully resolved using femtosecond XANES.

Solute-Solvent Charge-Transfer Excitations and Optical Absorption of Hydrated Hydroxide from Time-Dependent Density-Functional Theory.

PubMed

Opalka, Daniel; Sprik, Michiel

2014-06-10

The electronic structure of simple hydrated ions represents one of the most challenging problems in electronic-structure theory. Spectroscopic experiments identified the lowest excited state of the solvated hydroxide as a charge-transfer-to-solvent (CTTS) state. In the present work we report computations of the absorption spectrum of the solvated hydroxide ion, treating both solvent and solute strictly at the same level of theory. The average absorption spectrum up to 25 eV has been computed for samples taken from periodic ab initio molecular dynamics simulations. The experimentally observed CTTS state near the onset of the absorption threshold has been analyzed at the generalized-gradient approximation (GGA) and with a hybrid density-functional. Based on results for the lowest excitation energies computed with the HSE hybrid functional and a Davidson diagonalization scheme, the CTTS transition has been found 0.6 eV below the first absorption band of liquid water. The transfer of an electron to the solvent can be assigned to an excitation from the solute 2pπ orbitals, which are subject to a small energetic splitting due to the asymmetric solvent environment, to the significantly delocalized lowest unoccupied orbital of the solvent. The distribution of the centers of the excited state shows that CTTS along the OH(-) axis of the hydroxide ion is avoided. Furthermore, our simulations indicate that the systematic error arising in the calculated spectrum at the GGA originates from a poor description of the valence band energies in the solution.

Density gradient free electron collisionally excited x-ray laser

DOEpatents

Campbell, E.M.; Rosen, M.D.

1984-11-29

An operational x-ray laser is provided that amplifies 3p-3s transition x-ray radiation along an approximately linear path. The x-ray laser is driven by a high power optical laser. The driving line focused optical laser beam illuminates a free-standing thin foil that may be associated with a substrate for improved structural integrity. This illumination produces a generally cylindrically shaped plasma having an essentially uniform electron density and temperature, that exists over a long period of time, and provides the x-ray laser gain medium. The x-ray laser may be driven by more than one optical laser beam. The x-ray laser has been successfully demonstrated to function in a series of experimental tests.

Structural control of nonlinear optical absorption and refraction in dense metal nanoparticle arrays.

PubMed

Kohlgraf-Owens, Dana C; Kik, Pieter G

2009-08-17

The linear and nonlinear optical properties of a composite containing interacting spherical silver nanoparticles embedded in a dielectric host are studied as a function of interparticle separation using three dimensional frequency domain simulations. It is shown that for a fixed amount of metal, the effective third-order nonlinear susceptibility of the composite chi((3))(omega) can be significantly enhanced with respect to the linear optical properties, due to a combination of resonant surface plasmon excitation and local field redistribution. It is shown that this geometry-dependent susceptibility enhancement can lead to an improved figure of merit for nonlinear absorption. Enhancement factors for the nonlinear susceptibility of the composite are calculated, and the complex nature of the enhancement factors is discussed.

Electrons and Phonons in Semiconductor Multilayers

NASA Astrophysics Data System (ADS)

Ridley, B. K.

1996-11-01

This book provides a detailed description of the quantum confinement of electrons and phonons in semiconductor wells, superlattices and quantum wires, and shows how this affects their mutual interactions. It discusses the transition from microscopic to continuum models, emphasizing the use of quasi-continuum theory to describe the confinement of optical phonons and electrons. The hybridization of optical phonons and their interactions with electrons are treated, as are other electron scattering mechanisms. The book concludes with an account of the electron distribution function in three-, two- and one-dimensional systems, in the presence of electrical or optical excitation. This text will be of great use to graduate students and researchers investigating low-dimensional semiconductor structures, as well as to those developing new devices based on these systems.

Collisions between ultracold metastable He atoms

NASA Astrophysics Data System (ADS)

Woestenenk, G.; Mastwijk, H. C.; Thomsen, J. W.; vna der Straten, P.; Pieksma, M.; van Rijnbach, M.; Niehaus, A.

1999-06-01

We present experimental data on collisions between excited He-atoms occurring in a magneto-optical trap (MOT) at a temperature of 1.1 mK. He(2 3S)-atoms produced in a discharge are pre-cooled and trapped using the He(2 3S)-He(2 3P 2) transition for laser manipulation. Measurements of the Penning ionization rate as a function of the MOT-laser frequency are presented and theoretically analyzed. The analysis, based on a model which is presented in detail for the first time, leads to a good understanding of the complex nature of optical collisions. Further, first and preliminary measurements of the kinetic energy distributions of He 2+- and He +-ions formed by Penning ionization in optical collisions are presented.

Temperature-sensitive optrode

DOEpatents

Hirschfeld, T.B.

1985-09-24

Method and apparatus are provided for measuring temperature and for generating optical signals related to temperature. Light from a fiber optic is directed to a material whose fluorescent response varies with ambient temperature. The same fiber optic delivering the excitation beam also collects a portion of the fluorescent emission for analysis. Signal collection efficiency of the fiber optic is enhanced by requiring that the fluorescent probe material be in the shape of an oblong parabolically tapered solid. Reproducibility is enhanced by using Raman backscatter to monitor excitation beam fluctuations, and by using measurements of fluorescence lifetime. 10 figs.

Ultrashort optical waveguide excitations in uniaxial silica fibers: elastic collision scenarios.

PubMed

Kuetche, Victor K; Youssoufa, Saliou; Kofane, Timoleon C

2014-12-01

In this work, we investigate the dynamics of an uniaxial silica fiber under the viewpoint of propagation of ultimately ultrashort optical waveguide channels. As a result, we unveil the existence of three typical kinds of ultrabroadband excitations whose profiles strongly depend upon their angular momenta. Looking forward to surveying their scattering features, we unearth some underlying head-on scenarios of elastic collisions. Accordingly, we address some useful and straightforward applications in nonlinear optics through secured data transmission systems, as well as laser physics and soliton theory with optical soliton dynamics.

Temperature-sensitive optrode

DOEpatents

Hirschfeld, Tomas B.

1985-01-01

Method and apparatus are provided for measuring temperature and for generating optical signals related to temperature. Light from a fiber optic is directed to a material whose fluorescent response varies with ambient temperature. The same fiber optic delivering the excitation beam also collects a portion of the fluorescent emission for analysis. Signal collection efficiency of the fiber optic is enhanced by requiring that the fluorescent probe material be in the shape of an oblong parabolically tapered solid. Reproducibility is enhanced by using Raman backscatter to monitor excitation beam fluctuations, and by using measurements of fluorescence lifetime.

Laser scanning saturated structured illumination microscopy based on phase modulation

NASA Astrophysics Data System (ADS)

Huang, Yujia; Zhu, Dazhao; Jin, Luhong; Kuang, Cuifang; Xu, Yingke; Liu, Xu

2017-08-01

Wide-field saturated structured illumination microscopy has not been widely used due to the requirement of high laser power. We propose a novel method called laser scanning saturated structured illumination microscopy (LS-SSIM), which introduces high order of harmonics frequency and greatly reduces the required laser power for SSIM imaging. To accomplish that, an excitation PSF with two peaks is generated and scanned along different directions on the sample. Raw images are recorded cumulatively by a CCD detector and then reconstructed to form a high-resolution image with extended optical transfer function (OTF). Our theoretical analysis and simulation results show that LS-SSIM method reaches a resolution of 0.16 λ, equivalent to 2.7-fold resolution than conventional wide-field microscopy. In addition, LS-SSIM greatly improves the optical sectioning capability of conventional wide-field illumination system by diminishing our-of-focus light. Furthermore, this modality has the advantage of implementation in multi-photon microscopy with point scanning excitation to image samples in greater depths.

Retinal co-mediator acetylcholine evokes muscarinic inhibition of recurrent excitation in frog tectum column.

PubMed

Baginskas, Armantas; Kuras, Antanas

2016-08-26

Acetylcholine receptors contribute to the control of neuronal and neuronal network activity from insects to humans. We have investigated the action of acetylcholine receptors in the optic tectum of Rana temporaria (common frog). Our previous studies have demonstrated that acetylcholine activates presynaptic nicotinic receptors, when released into the frog optic tectum as a co-mediator during firing of a single retinal ganglion cell, and causes: a) potentiation of retinotectal synaptic transmission, and b) facilitation of transition of the tectum column to a higher level of activity. In the present study we have shown that endogenous acetylcholine also activates muscarinic receptors, leading to a delayed inhibition of recurrent excitatory synaptic transmission in the tectum column. The delay of muscarinic inhibition was evaluated to be of ∼80ms, with an extent of inhibition of ∼2 times. The inhibition of the recurrent excitation determines transition of the tectum column back to its resting state, giving a functional sense for the inhibition. Copyright © 2016 Elsevier Ireland Ltd. All rights reserved.

All-Optical Electrophysiology for Disease Modeling and Pharmacological Characterization of Neurons.

PubMed

Werley, Christopher A; Brookings, Ted; Upadhyay, Hansini; Williams, Luis A; McManus, Owen B; Dempsey, Graham T

2017-09-11

A key challenge for establishing a phenotypic screen for neuronal excitability is measurement of membrane potential changes with high throughput and accuracy. Most approaches for probing excitability rely on low-throughput, invasive methods or lack cell-specific information. These limitations stimulated the development of novel strategies for characterizing the electrical properties of cultured neurons. Among these was the development of optogenetic technologies (Optopatch) that allow for stimulation and recording of membrane voltage signals from cultured neurons with single-cell sensitivity and millisecond temporal resolution. Neuronal activity is elicited using blue light activation of the channelrhodopsin variant 'CheRiff'. Action potentials and synaptic signals are measured with 'QuasAr', a rapid and sensitive voltage-indicating protein with near-infrared fluorescence that scales proportionately with transmembrane potential. This integrated technology of optical stimulation and recording of electrical signals enables investigation of neuronal electrical function with unprecedented scale and precision. © 2017 by John Wiley & Sons, Inc. Copyright © 2017 John Wiley & Sons, Inc.

Multiple protocol fluorometer and method

DOEpatents

Kolber, Zbigniew S.; Falkowski, Paul G.

2000-09-19

A multiple protocol fluorometer measures photosynthetic parameters of phytoplankton and higher plants using actively stimulated fluorescence protocols. The measured parameters include spectrally-resolved functional and optical absorption cross sections of PSII, extent of energy transfer between reaction centers of PSII, F.sub.0 (minimal), F.sub.m (maximal) and F.sub.v (variable) components of PSII fluorescence, photochemical and non-photochemical quenching, size of the plastoquinone (PQ) pool, and the kinetics of electron transport between Q.sub.a and PQ pool and between PQ pool and PSI. The multiple protocol fluorometer, in one embodiment, is equipped with an excitation source having a controlled spectral output range between 420 nm and 555 nm and capable of generating flashlets having a duration of 0.125-32 .mu.s, an interval between 0.5 .mu.s and 2 seconds, and peak optical power of up to 2 W/cm.sup.2. The excitation source is also capable of generating, simultaneous with the flashlets, a controlled continuous, background illumination.

Characterization of the intramolecular transfer state of marine carotenoid fucoxanthin by femtosecond pump-probe spectroscopy.

PubMed

Kosumi, Daisuke; Fujii, Ritsuko; Sugisaki, Mitsuru; Oka, Naohiro; Iha, Masahiko; Hashimoto, Hideki

2014-07-01

Fucoxanthin, containing a carbonyl group in conjugation with its polyene backbone, is a naturally occurring pigment in marine organisms and is essential to the photosynthetic light-harvesting function in brown alga and diatom. Fucoxanthin exhibits optical characteristics attributed to an intramolecular charge transfer (ICT) state that arises in polar environments due to the presence of the carbonyl group. In this study, we report the spectroscopic properties of fucoxanthin in methanol (polar and protic solvent) observed by femtosecond pump-probe measurements in the near-infrared region, where transient absorption associated with the optically allowed S2 (1(1)B u (+) ) state and stimulated emission from the strongly coupled S1/ICT state were observed following one-photon excitation to the S2 state. The results showed that the amplitude of the stimulated emission of the S1/ICT state increased with decreasing excitation energy, demonstrating that the fucoxanthin form associated with the lower energy of the steady-state absorption exhibits stronger ICT character.

Twistacene contained molecule for optical nonlinearity: Excited-state based negative refraction and optical limiting

NASA Astrophysics Data System (ADS)

Wu, Xingzhi; Xiao, Jinchong; Sun, Ru; Jia, Jidong; Yang, Junyi; Ao, Guanghong; Shi, Guang; Wang, Yuxiao; Zhang, Xueru; Song, Yinglin

2018-06-01

Spindle-type molecules containing twisted acenes (PyBTA-1 &PyBTA-2) are designed, synthesized characterized. Picosecond Z-scan experiments under 532 nm show reverse saturable absorption and negative nonlinear refraction, indicating large third-order optical nonlinearity in PyBTA-1. The mechanism of the optical nonlinearity is investigated and the results show that the nonlinear absorption and refraction in PyBTA-1 originates from a charge transfer (CT) state. Furthermore, relatively long lifetime and absorptive cross section of the CT state are measured. Based on the excited state absorption in PyBTA-1, strong optical limiting with ∼0.3 J/cm2 thresholds are obtained when excited by picoseconds and nanoseconds pulses. The findings on nonlinear optics suggest PyBTA-1 a promising material of all optical modulation and laser protection, which enrich the potential applications of these spindle-type molecules. Comparing to the previously reported spindle-type molecules with analogous structures, the introduction of ICT in PyBTA-1 &PyBTA-2 dramatically decreases the two-photon absorption while enhances the nonlinear refraction. The results could be used to selectively tailor the optical nonlinearity in such kind of compounds.

Non-linear optical response by functionalized gold nanospheres: identifying design principles to maximize the molecular photo-release.

PubMed

Bergamini, Luca; Voliani, Valerio; Cappello, Valentina; Nifosì, Riccardo; Corni, Stefano

2015-08-28

In a recent study by Voliani et al. [Small, 2011, 7, 3271], the electromagnetic field enhancement in the vicinity of the gold nanoparticle surface has been exploited to achieve photocontrolled release of a molecular cargo conjugated to the nanoparticles via 1,2,3-triazole, a photocleavable moiety. The aim of the present study is to investigate the mechanism of the photorelease by characterizing the nanoparticle aggregation status within the cells and simulating the electric field enhancement in a range of experimentally realistic geometries, such as single Au nanoparticles, dimers, trimers and random aggregates. Two plasmon-enhanced processes are examined for triazole photocleavage, i.e. three-photon excitation and third-harmonic-generation (one-photon) excitation. Taking into account the absorption cross sections of the triazole, we conclude that the latter mechanism is more efficient, and provides a photocleavage rate that explains the experimental findings. Moreover, we determine which aggregate geometries are required to maximize the field enhancement, and the dependence of such enhancement on the excitation wavelength. Our results provide design principles for maximizing the multiphoton molecular photorelease by such functionalized gold nanoparticles.

Monte Carlo modeling of fluorescence in semi-infinite turbid media

NASA Astrophysics Data System (ADS)

Ong, Yi Hong; Finlay, Jarod C.; Zhu, Timothy C.

2018-02-01

The incident field size and the interplay of absorption and scattering can influence the in-vivo light fluence rate distribution and complicate the absolute quantification of fluorophore concentration in-vivo. In this study, we use Monte Carlo simulations to evaluate the effect of incident beam radius and optical properties to the fluorescence signal collected by isotropic detector placed on the tissue surface. The optical properties at the excitation and emission wavelengths are assumed to be identical. We compute correction factors to correct the fluorescence intensity for variations due to incident field size and optical properties. The correction factors are fitted to a 4-parameters empirical correction function and the changes in each parameter are compared for various beam radius over a range of physiologically relevant tissue optical properties (μa = 0.1 - 1 cm-1 , μs'= 5 - 40 cm-1 ).

Optical absorption by indirect excitons in a transition metal dichalcogenide/hexagonal boron nitride heterostructure

NASA Astrophysics Data System (ADS)

Brunetti, Matthew N.; Berman, Oleg L.; Kezerashvili, Roman Ya

2018-06-01

We study optical transitions in spatially indirect excitons in transition metal dichalcogenide (TMDC) heterostructures separated by an integer number of hexagonal boron nitride (h-BN) monolayers. By solving the Schrödinger equation with the Keldysh potential for a spatially indirect exciton, we obtain eigenfunctions and eigenenergies for the ground and excited states and study their dependence on the interlayer separation, controlled by varying the number of h-BN monolayers. The oscillator strength, optical absorption coefficient, and optical absorption factor, the fraction of incoming photons absorbed in the TMDC/h-BN/TMDC heterostructure, are evaluated and studied as a function of the interlayer separation. Using input parameters from the existing literature which give the largest and the smallest spatially indirect exciton binding energy, we provide upper and lower bounds on all quantities presented.

High resolution multiplexed functional imaging in live embryos (Conference Presentation)

NASA Astrophysics Data System (ADS)

Xu, Dongli; Zhou, Weibin; Peng, Leilei

2017-02-01

Fourier multiplexed fluorescence lifetime imaging (FmFLIM) scanning laser optical tomography (FmFLIM-SLOT) combines FmFLIM and Scanning laser optical tomography (SLOT) to perform multiplexed 3D FLIM imaging of live embryos. The system had demonstrate multiplexed functional imaging of zebrafish embryos genetically express Foster Resonant Energy Transfer (FRET) sensors. However, previous system has a 20 micron resolution because the focused Gaussian beam diverges quickly from the focused plane, makes it difficult to achieve high resolution imaging over a long projection depth. Here, we present a high-resolution FmFLIM-SLOT system with achromatic Bessel beam, which achieves 3 micron resolution in 3D deep tissue imaging. In Bessel-FmFLIM-SLOT, multiple laser excitation lines are firstly intensity modulated by a Michelson interferometer with a spinning polygon mirror optical delay line, which enables Fourier multiplexed multi-channel lifetime measurements. Then, a spatial light modulator and a prism are used to transform the modulated Gaussian laser beam to an achromatic Bessel beam. The achromatic Bessel beam scans across the whole specimen with equal angular intervals as sample rotated. After tomography reconstruction and the frequency domain lifetime analysis method, both the 3D intensity and lifetime image of multiple excitation-emission can be obtained. Using Bessel-FmFLIM-SLOT system, we performed cellular-resolution FLIM tomography imaging of live zebrafish embryo. Genetically expressed FRET sensors in these embryo will allow non-invasive observation of multiple biochemical processes in vivo.

Physical and optical properties of calcium sulfate ultra-phosphate glass-doped Er2O3

NASA Astrophysics Data System (ADS)

Aliyu, Aliyu Mohammed; Hussin, R.; Deraman, Karim; Ahmad, N. E.; Danmadami, Amina M.; Yamusa, Y. A.

2018-03-01

The influence of erbium on physical and optical properties of calcium sulfate ultra-phosphate glass was investigated using conventional melt quench process. Selected samples of composition 20CaSO4 (80 - x) P2O5- xEr2O3 with 0.1 ≤x ≤ 0.9 mol.% were prepared and assessed. X-ray diffraction (XRD) techniques were used to confirm the amorphous nature of the said samples. The structural units of phosphate-based glass were assessed from Raman spectra as ultra-(Q3), meta-(Q2), pyro-(Q1) and orthophosphate (Q0) units. Depolymerization process of the glasses was testified for higher calcium oxide content and UV-visible for optical measurement. Thermal analysis have been investigated by means of thermogravimetric analysis. The results show the decomposition of materials in the temperature range of 25∘C-1000∘C. Er3+ absorption spectra were measured in the range of 400-1800nm. PL measurement was carried out in order to obtain the excitation and emission spectra of the samples. The emission spectra excited at 779nm comprises of 518nm, 550nm and 649nm of transition 4F9/2, 4S3/2 and 2H11/2 excited states to 4I15/2 ground state. In physical properties, the density calculated using Archimedes method is inversely proportional to molar volume with increase in Er3+ ions. Optical bandgap (Eg) were determined using Tauc’s plots for direct transitions where Eg (direct) decreases with increase in erbium content. The refractive index increases with decreasing molar volume; this may have a tendency for larger optical bandgap. The result obtained from the glass matrix indicates that erbium oxide-doped calcium sulfate ultra-phosphate may give important information for wider development of functional glasses.

Valence and charge-transfer optical properties for some SinCm (m, n ≤ 12) clusters: Comparing TD-DFT, complete-basis-limit EOMCC, and benchmarks from spectroscopy.

PubMed

Lutz, Jesse J; Duan, Xiaofeng F; Ranasinghe, Duminda S; Jin, Yifan; Margraf, Johannes T; Perera, Ajith; Burggraf, Larry W; Bartlett, Rodney J

2018-05-07

Accurate optical characterization of the closo-Si 12 C 12 molecule is important to guide experimental efforts toward the synthesis of nano-wires, cyclic nano-arrays, and related array structures, which are anticipated to be robust and efficient exciton materials for opto-electronic devices. Working toward calibrated methods for the description of closo-Si 12 C 12 oligomers, various electronic structure approaches are evaluated for their ability to reproduce measured optical transitions of the SiC 2 , Si 2 C n (n = 1-3), and Si 3 C n (n = 1, 2) clusters reported earlier by Steglich and Maier [Astrophys. J. 801, 119 (2015)]. Complete-basis-limit equation-of-motion coupled-cluster (EOMCC) results are presented and a comparison is made between perturbative and renormalized non-iterative triples corrections. The effect of adding a renormalized correction for quadruples is also tested. Benchmark test sets derived from both measurement and high-level EOMCC calculations are then used to evaluate the performance of a variety of density functionals within the time-dependent density functional theory (TD-DFT) framework. The best-performing functionals are subsequently applied to predict valence TD-DFT excitation energies for the lowest-energy isomers of Si n C and Si n-1 C 7-n (n = 4-6). TD-DFT approaches are then applied to the Si n C n (n = 4-12) clusters and unique spectroscopic signatures of closo-Si 12 C 12 are discussed. Finally, various long-range corrected density functionals, including those from the CAM-QTP family, are applied to a charge-transfer excitation in a cyclic (Si 4 C 4 ) 4 oligomer. Approaches for gauging the extent of charge-transfer character are also tested and EOMCC results are used to benchmark functionals and make recommendations.

Multi-color autofluorescence and scattering spectroscopy provides rapid assessment of kidney function following ischemic injury

NASA Astrophysics Data System (ADS)

Raman, Rajesh N.; Pivetti, Chris D.; Ramsamooj, Rajendra; Troppmann, Christoph; Demos, Stavros G.

2018-02-01

A major source of kidneys for transplant comes from deceased donors whose tissues have suffered an unknown amount of warm ischemia prior to retrieval, with no quantitative means to assess function before transplant. Toward addressing this need, non-contact monitoring of optical signatures in rat kidneys was performed in vivo during ischemia and reperfusion. Kidney autofluorescence images were captured under ultraviolet illumination (355 nm, 325 nm, and 266 nm) in order to provide information on related metabolic and non-metabolic response. In addition, light scattering images under 355 nm, 325 nm, and 266 nm, 500 nm illumination were monitored to report on changes in kidney optical properties giving rise to the observed autofluorescence signals during these processes. During reperfusion, various signal ratios were generated from the recorded signals and then parametrized. Time-dependent parameters derived from the ratio of autofluorescence under 355 nm excitation to that under 266 nm excitation, as well as from 500 nm scattered signal, were found capable of discriminating dysfunctional kidneys from those that were functional (p < 0.01) within hours of reperfusion. Kidney dysfunction was confirmed by subsequent survival study and histology following autopsy up to a week later. Physiologic changes potentially giving rise to the observed signals, including those in cellular metabolism, vascular response, tissue microstructure, and microenvironment chemistry, are discussed.

Edge-on and face-on functionalized Pc on enriched semiconducting SWCNT hybrids.

PubMed

Arellano, Luis M; Martín-Gomis, Luis; Gobeze, Habtom B; Molina, Desiré; Hermosa, Cristina; Gómez-Escalonilla, María J; Fierro, José Luis G; Sastre-Santos, Ángela; D'Souza, Francis; Langa, Fernando

2018-03-15

Enriched semiconducting single-walled carbon nanotubes (SWCNT (6,5) and SWCNT (7,6)) and HiPco nanotubes were covalently functionalized with either zinc phthalocyanine or silicon phthalocyanine as electron donors. The synthetic strategy resulted in edge-on and face-on geometries with respect to the phthalocyanine geometry, with both phthalocyanines held by an electronically conducting diphenylacetylene linker. The extent of functionalization in the MPc-SWCNT (M = Zn or Si) donor-acceptor nanohybrids was determined by systematic studies involving AFM, TGA, XPS, optical and Raman techniques. Intramolecular interactions in MPc-SWCNT nanohybrids were probed by studies involving optical absorbance, Raman, luminescence and electrochemical studies. Different degrees of interactions were observed depending on the type of MPc and mode of attachment. Substantial quenching of MPc fluorescence in these hybrids was observed from steady-state and three-dimensional fluorescence mapping, which suggests the occurrence of excited state events. Evidence for the occurrence of excited state charge transfer type interactions was subsequently secured from femtosecond transient absorption studies covering both the visible and near-infrared regions. Furthermore, electron-pooling experiments performed in the presence of a sacrificial electron donor and a second electron acceptor revealed accumulation of one-electron reduced product upon continuous irradiation of the nanohybrids. In such experiments, the ZnPc-SWCNT (6,5) nanohybrid outperformed other nanohybrids and this suggests that this is a superior donor-acceptor system for photocatalytic applications.

Exploring Photoinduced Excited State Evolution in Heterobimetallic Ru(II)-Co(III) Complexes.

PubMed

Kuhar, Korina; Fredin, Lisa A; Persson, Petter

2015-06-18

Quantum chemical calculations provide detailed theoretical information concerning key aspects of photoinduced electron and excitation transfer processes in supramolecular donor-acceptor systems, which are particularly relevant to fundamental charge separation in emerging molecular approaches for solar energy conversion. Here we use density functional theory (DFT) calculations to explore the excited state landscape of heterobimetallic Ru-Co systems with varying degrees of interaction between the two metal centers, unbound, weakly bound, and tightly bound systems. The interplay between structural and electronic factors involved in various excited state relaxation processes is examined through full optimizations of multiple charge/spin states of each of the investigated systems. Low-energy relaxed heterobimetallic states of energy transfer and excitation transfer character are characterized in terms of energy, structure, and electronic properties. These findings support the notion of efficient photoinduced charge separation from a Ru(II)-Co(III) ground state, via initial optical excitation of the Ru-center, to low-energy Ru(III)-Co(II) states. The strongly coupled system has significant involvement of the conjugated bridge, qualitatively distinguishing it from the other two weakly coupled systems. Finally, by constructing potential energy surfaces for the three systems where all charge/spin state combinations are projected onto relevant reaction coordinates, excited state decay pathways are explored.

Excitation of plasmonic waves in metal-dielectric structures by a laser beam using holography principles

NASA Astrophysics Data System (ADS)

Ignatov, A. I.; Merzlikin, A. M.

2018-03-01

A method for development of gratings for effective excitation of surface plasmonic waves using holography principles has been proposed and theoretically analyzed. For the case of a plasmonic wave in a dielectric layer on metal, the proposed volume hologram is 1.7 times more effective than the simple grating of slits in the dielectric layer with the optimized period and slits' width. The advantage of the hologram over the optimized grating is in the refractive index distribution that accounts phase relationships between an exciting and an excited waves more correctly. The proposed holographic method is universal. As expected, this can be extended for effective excitation of different types of optical surface waves and modes of optical waveguides.

Nano-cone optical fiber array sensors for MiRNA profiling

NASA Astrophysics Data System (ADS)

Wang, Yunshan; Senapati, Satyajyoti; Stoddart, Paul; Howard, Scott; Chang, Hsueh-Chia

2013-09-01

Up/down regulation of microRNA panels has been correlated to cardiovascular diseases and cancer. Frequent miRNA profiling at home can hence allow early cancer diagnosis and home-use chronic disease monitoring, thus reducing both mortality rate and healthcare cost. However, lifetime of miRNAs is less than 1 hour without preservation and their concentrations range from pM to mM. Despite rapid progress in the last decade, modern nucleic acid analysis methods still do not allow personalized miRNA profiling---Real-time PCR and DNA micro-array both require elaborate miRNA preservation steps and expensive equipment and nano pore sensors cannot selectively quantify a large panel with a large dynamic range. We report a novel and low-cost optical fiber sensing platform, which has the potential to profile a panel of miRNA with simple LED light sources and detectors. The individual tips of an optical imaging fiber bundle (mm in diameter with 7000 fiber cores) were etched into cones with 10 nm radius of curvature and coated with Au. FRET (Forster Resonant Energy Transfer) hairpin oligo probes, with the loop complementary to a specific miRNA that can release the hairpin, were functionalized onto the conic tips. Exciting light in the optical fiber waveguide is optimally coupled to surface plasmonics on the gold surface, which then converges to the conic tips with two orders of magnitude enhancement in intensity. Unlike nanoparticle plasmonics, tip plasmonics can be excited over a large band width and hence the plasmonic enhanced fluorescence signal of the FRET reporter is also focused towards the tip--- and is further enhanced with the periodic resonant grid of the fiber array which gives rise to pronounced standing wave interference patterns. Multiplexing is realized by functionalizing different probes onto one fiber bundle using a photoactivation process.

Advances in functional X-ray imaging techniques and contrast agents

PubMed Central

Chen, Hongyu; Rogalski, Melissa M.

2012-01-01

X-rays have been used for non-invasive high-resolution imaging of thick biological specimens since their discovery in 1895. They are widely used for structural imaging of bone, metal implants, and cavities in soft tissue. Recently, a number of new contrast methodologies have emerged which are expanding X-ray’s biomedical applications to functional as well as structural imaging. These techniques are promising to dramatically improve our ability to study in situ biochemistry and disease pathology. In this review, we discuss how X-ray absorption, X-ray fluorescence, and X-ray excited optical luminescence can be used for physiological, elemental, and molecular imaging of vasculature, tumours, pharmaceutical distribution, and the surface of implants. Imaging of endogenous elements, exogenous labels, and analytes detected with optical indicators will be discussed. PMID:22962667

X-Ray Sum Frequency Diffraction for Direct Imaging of Ultrafast Electron Dynamics

NASA Astrophysics Data System (ADS)

Rouxel, Jérémy R.; Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul

2018-06-01

X-ray diffraction from molecules in the ground state produces an image of their charge density, and time-resolved x-ray diffraction can thus monitor the motion of the nuclei. However, the density change of excited valence electrons upon optical excitation can barely be monitored with regular diffraction techniques due to the overwhelming background contribution of the core electrons. We present a nonlinear x-ray technique made possible by novel free electron laser sources, which provides a spatial electron density image of valence electron excitations. The technique, sum frequency generation carried out with a visible pump and a broadband x-ray diffraction pulse, yields snapshots of the transition charge densities, which represent the electron density variations upon optical excitation. The technique is illustrated by ab initio simulations of transition charge density imaging for the optically induced electronic dynamics in a donor or acceptor substituted stilbene.

Damping of Bogoliubov excitations in optical lattices

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

Tsuchiya, Shunji; Department of Physics, Waseda University, 3-4-1 Okubo, Tokyo 169-8555; Griffin, Allan

2004-08-01

Extending recent work to finite temperatures, we calculate the Landau damping of a Bogoliubov excitation in an optical lattice, due to the coupling to a thermal cloud of such excitations. For simplicity, we consider a one-dimensional Bose-Hubbard model and restrict ourselves to the first energy band. For energy conservation to be satisfied, the excitations in the collision processes must exhibit ''anomalous dispersion,'' analogous to phonons in superfluid {sup 4}He. This leads to the disappearance of all damping processes when Un{sup c0}{>=}6J, where U is the on-site interaction, J is the hopping matrix element, and n{sup c0}(T) is the number ofmore » condensate atoms at a lattice site. This phenomenon also occurs in two-dimensional and three-dimensional optical lattices. The disappearance of Beliaev damping above a threshold wave vector is noted.« less

Effect of Intense Optical Excitation on Internal Electric Field Evolution in CdTe Gamma-Ray Detectors

NASA Astrophysics Data System (ADS)

Suzuki, K.; Ichinohe, Y.; Seto, S.

2018-03-01

The time-of-flight (TOF) transient currents in radiation detectors made of CdTe and Cd0.9Zn0.1Te (CZT) have been measured at several optical excitation intensities to investigate the effect of drifting carriers on the internal field. Both detectors show so-called space-charge-perturbed (SCP) current under intense optical excitation. A Monte Carlo (MC) simulation combined with an iterative solution of Poisson's equation is used to reproduce the observed currents under several bias voltages and excitation intensities. The SCP theory describes well the transient current in the CZT detector, whereas injection of holes from the anode and a corresponding reduction of the electron lifetime are further required to describe that in the CdTe detector. We visualize the temporal changes in the charge distribution and internal electric field profiles of both detectors.

Selective laser spectroscopy of molecules and ions in solids: a history, fundamentals and applications

NASA Astrophysics Data System (ADS)

Sapozhnikov, Michael

2018-03-01

A history of the development of selective laser spectroscopy is presented, beginning with a pioneering work by Yu. V. Denisov and V. A. Kizel in 1967, who were the first to demonstrate the possibility of removing the inhomogeneous broadening of luminescence spectra of impurity ions in glasses upon monochromatic resonance excitation. Selective excitation of optical centers can be achieved due to existence of zero-phonon transitions corresponding to narrow homogeneous zero-phonon lines in the spectra of impurity centers in solids, which are hidden in broad inhomogeneous optical bands upon usual nonselective excitation. The fundamentals of zero-phonon transition spectroscopy are considered and the mechanism of removing the inhomogeneous broadening of optical spectra of ions and molecules in crystals and amorphous solids under selective laser excitation of luminescence and persistent hole burning in absorption spectra is presented in detail. Various applications of selective laser spectroscopy for fundamental and applied studies are discussed.

Many-body perturbation theory for understanding optical excitations in organic molecules and solids

NASA Astrophysics Data System (ADS)

Sharifzadeh, Sahar

2018-04-01

Semiconductors composed of organic molecules are promising as components for flexible and inexpensive optoelectronic devices, with many recent studies aimed at understanding their electronic and optical properties. In particular, computational modeling of these complex materials has provided new understanding of the underlying properties which give rise to their excited-state phenomena. This article provides an overview of recent many-body perturbation theory (MBPT) studies of optical excitations within organic molecules and solids. We discuss the accuracy of MBPT within the GW/BSE approach in predicting excitation energies and absorption spectra, and assess the impact of two commonly used approximations, the DFT starting point and the Tamm–Dancoff approximation. Moreover, we summarize studies that elucidate the role of solid-state structure on the nature of excitons in organic crystals. These studies show that a rich physical understanding of organic materials can be obtained from GW/BSE.

Electron impact excitation of the electronic states of N2. III - Transitions in the 12.5-14.2-eV energy-loss region at incident energies of 40 and 60 eV

NASA Technical Reports Server (NTRS)

Chutjian, A.; Trajmar, S.; Cartwright, D. C.

1977-01-01

Analysis of electron energy-loss data at incident electron energies of 40 and 60 eV has led to the determination of normalized absolute differential cross sections for electron-impact excitation of five optically-allowed singlet states, two known triplet states, and two unknown triplet-like states of N2, lying in the energy-loss range 12.5-14.2 eV. The range of scattering angles was 5 to 138 deg. The optically allowed transitions and the known triplet excitations are identified. Cross sections for excitation to two unidentified triplet-like states at 13.155 and 13.395 eV were also obtained. The relationship of the generalized oscillator strength for the dipole-allowed states obtained from the described data to known optical oscillator strengths is discussed.

Basic optical and radiation response properties of Lumilass-B fluorescent glass

NASA Astrophysics Data System (ADS)

Fujimoto, Yutaka; Yanagida, Takayuki

2014-08-01

The optical, scintillation, and dosimetric properties of Lumilass-B fluorescent glass were studied. The glass showed an ultraviolet absorption band that can be attributed to the transition from 4f7(8S7/2) ground state to the 4f65d excited state of Eu2+ ions in the glass matrix. When an X-ray excited the glass, the radioluminescence band appeared at 400 nm as in the PL spectrum. This is identified as the transition from the 5d excited state to the 4f7(8S7/2) ground state of Eu2+. The scintillation decay time under excitation with the pulsed X-ray was calculated to be about 630 ns. The irradiation dose response of the thermoluminescence (TL) and optically-stimulated luminescence (OSL) intensities was linear in the studied dose range at 0.25-200 mGy and 0.25-16 Gy, respectively.

In-vivo multi-nonlinear optical imaging of a living cell using a supercontinuum light source generated from a photonic crystal fiber

NASA Astrophysics Data System (ADS)

Kano, Hideaki; Hamaguchi, Hiro-O.

2006-04-01

A supercontinuum light source generated with a femtosecond Ti:Sapphire oscillator has been used to obtain both vibrational and two-photon excitation fluorescence (TPEF) images of a living cell simultaneously at different wavelengths. Owing to an ultrabroadband spectral profile of the supercontinuum, multiple vibrational resonances have been detected through coherent anti-Stokes Raman scattering (CARS) process. In addition to the multiplex CARS process, multiple electronic states can be excited due to the broadband electronic two-photon excitation using the supercontinuum, giving rise to a two-photon excitation fluorescence (TPEF) signal. Using a living yeast cell whose nucleus is labeled by green fluorescent protein (GFP), we have succeeded in visualizing organelles such as mitochondria, septum, and nucleus through the CARS and the TPEF processes. The supercontinuum enables us to perform unique multi-nonlinear optical imaging through two different nonlinear optical processes.

Preliminary study of diagnostic spectroscopic imaging for nasopharyngeal carcinoma

NASA Astrophysics Data System (ADS)

Li, Buhong; Xie, Shusen; Zhang, Xiaodong; Li, Depin

2003-12-01

The optical biopsy system for nasopharyngeal carcinoma based on the technique of laser-induced exogenous fluorescence has been successful developed. Ar+ laser was selected as the excitation light source based on the measurement of the Emission-Excitation Matrix of Hematoporphyrin Monomethyl Ether. Tissue-simulating optical phantoms diluted with different concentration of HMME were used to simulated nasopharyngeal carcinoma lesions in the performance test for the drug-fluorescence optical biopsy system, especially for the comparison of fluorescence image contrast between the excitation wavelength of 488nm and 514.5nm, respectively. Experimental results show that the fluorescence image contrast of simulated nasopharyngeal carcinoma lesions excited by the light at the wavelength of 488nm is about three fold higher than that at 514.5nm, and the sensitivity and resolution of the fluorescence and reflection twilight image can satisfy the needs for clinical diagnosis and localization.

Terahertz pulse generation by the tilted pulse front technique using an M-shaped optical system

NASA Astrophysics Data System (ADS)

Morita, Ken; Shiozawa, Kento; Suizu, Koji; Ishitani, Yoshihiro

2018-05-01

To achieve the phase matching condition in terahertz (THz) pulse generation by the tilted pulse front technique, it is necessary to rebuild the entire optical setup if the optical conditions, such as excitation wavelength, temperature of nonlinear crystal, and output THz frequency, are changed. We propose THz pulse generation by the tilted pulse front technique using an M-shaped configuration. This system allows us to change the optical conditions only by tuning a few optics and without rebuilding the entire setup. We change the excitation wavelength at a fixed radiation frequency and assess the performance of the proposed system.

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

Kertzscher, G; Beddar, S

Purpose: To study the promising potential of inorganic scintillator detectors (ISDs) and investigate various unwanted luminescence properties which may compromise their accuracy. Methods: The ISDs were comprised of a ruby crystal coupled to a polymethyl methacrylate (PMMA) fiber-optic cable and a charged coupled device camera. A new type of ISD was manufactured and included a long-pass filter that was sandwiched between the crystal and the fiber-optic cable. The purpose of the filter was to suppress the Cerenkov and fluorescence background light induced in the PMMA (the stem signal) from striking the ruby crystal, generating unwanted ruby excitation. A variety ofmore » experiments were performed to characterize the ruby based ISDs. The relative contribution of the induced ruby signal and the stem signal were quantified while exposing the detector and a bare fiber-optic cable to a high dose rate (HDR) brachytherapy (BT) source, respectively. The unwanted ruby excitation was quantified while irradiating the fiber-optic cable with the detector volume shielded. Other experiments addressed time-dependent luminescence properties and a comparison to other commonly used organic scintillator detectors (BCF-12, BCF-60). Results: When the BT source dwelled 0.5 cm away from the fiber-optic cable, the unwanted ruby excitation amounted to >5% of the total signal if the source-distance from the scintillator was >7 cm. However, the unwanted excitation was suppressed to <1% if the ISD incorporated an optic filter. The stem signal was suppressed with a 20 nm band-pass filter and was <3% as long as the source-distance was <7 cm. The ruby based ISDs generated signal up to 20(40) times that of BCF-12(BCF-60). Conclusion: The study presents solutions to unwanted luminescence properties of ruby based ISDs for HDR BT. An optic filter should be sandwiched between the scintillator volume and the fiber-optic cable to prevent the stem signal to excite the ruby crystal.« less

Theoretical description of protein field effects on electronic excitations of biological chromophores.

PubMed

Varsano, Daniele; Caprasecca, Stefano; Coccia, Emanuele

2017-01-11

Photoinitiated phenomena play a crucial role in many living organisms. Plants, algae, and bacteria absorb sunlight to perform photosynthesis, and convert water and carbon dioxide into molecular oxygen and carbohydrates, thus forming the basis for life on Earth. The vision of vertebrates is accomplished in the eye by a protein called rhodopsin, which upon photon absorption performs an ultrafast isomerisation of the retinal chromophore, triggering the signal cascade. Many other biological functions start with the photoexcitation of a protein-embedded pigment, followed by complex processes comprising, for example, electron or excitation energy transfer in photosynthetic complexes. The optical properties of chromophores in living systems are strongly dependent on the interaction with the surrounding environment (nearby protein residues, membrane, water), and the complexity of such interplay is, in most cases, at the origin of the functional diversity of the photoactive proteins. The specific interactions with the environment often lead to a significant shift of the chromophore excitation energies, compared with their absorption in solution or gas phase. The investigation of the optical response of chromophores is generally not straightforward, from both experimental and theoretical standpoints; this is due to the difficulty in understanding diverse behaviours and effects, occurring at different scales, with a single technique. In particular, the role played by ab initio calculations in assisting and guiding experiments, as well as in understanding the physics of photoactive proteins, is fundamental. At the same time, owing to the large size of the systems, more approximate strategies which take into account the environmental effects on the absorption spectra are also of paramount importance. Here we review the recent advances in the first-principle description of electronic and optical properties of biological chromophores embedded in a protein environment. We show their applications on paradigmatic systems, such as the light-harvesting complexes, rhodopsin and green fluorescent protein, emphasising the theoretical frameworks which are of common use in solid state physics, and emerging as promising tools for biomolecular systems.

Theoretical description of protein field effects on electronic excitations of biological chromophores

NASA Astrophysics Data System (ADS)

Varsano, Daniele; Caprasecca, Stefano; Coccia, Emanuele

2017-01-01

Photoinitiated phenomena play a crucial role in many living organisms. Plants, algae, and bacteria absorb sunlight to perform photosynthesis, and convert water and carbon dioxide into molecular oxygen and carbohydrates, thus forming the basis for life on Earth. The vision of vertebrates is accomplished in the eye by a protein called rhodopsin, which upon photon absorption performs an ultrafast isomerisation of the retinal chromophore, triggering the signal cascade. Many other biological functions start with the photoexcitation of a protein-embedded pigment, followed by complex processes comprising, for example, electron or excitation energy transfer in photosynthetic complexes. The optical properties of chromophores in living systems are strongly dependent on the interaction with the surrounding environment (nearby protein residues, membrane, water), and the complexity of such interplay is, in most cases, at the origin of the functional diversity of the photoactive proteins. The specific interactions with the environment often lead to a significant shift of the chromophore excitation energies, compared with their absorption in solution or gas phase. The investigation of the optical response of chromophores is generally not straightforward, from both experimental and theoretical standpoints; this is due to the difficulty in understanding diverse behaviours and effects, occurring at different scales, with a single technique. In particular, the role played by ab initio calculations in assisting and guiding experiments, as well as in understanding the physics of photoactive proteins, is fundamental. At the same time, owing to the large size of the systems, more approximate strategies which take into account the environmental effects on the absorption spectra are also of paramount importance. Here we review the recent advances in the first-principle description of electronic and optical properties of biological chromophores embedded in a protein environment. We show their applications on paradigmatic systems, such as the light-harvesting complexes, rhodopsin and green fluorescent protein, emphasising the theoretical frameworks which are of common use in solid state physics, and emerging as promising tools for biomolecular systems.

Structure Effect of Squarylium Cyanine Dyes on Third-Order Optical Nonlinearities in Ground and Excited States

NASA Astrophysics Data System (ADS)

Liu, Xu-chun; Xu, Gang; Si, Jin-hai; Ye, Pei-xian; Lin, Tong; Peng, Bi-xian

1999-08-01

A series of squarylium cyanine dyes with different substituents were synthesized and the third-order optical nonlinearities of their ground and excited states were investigated by backward degenerate four-wave-mixing. For the ground state, the molecular hyperpolarizability γg increases with the red-shift of the absorption peak λmaxab of the squaraine with different substituents, whereas for the excited-state molecular hyperpolarizability γe, the nonlinear enhancement γe/γg decreases, which may indicate that in the excited state the electron accepting-donating ability of different substituents changes in the reverse order compared with the order in the ground state.

Electronic and optical properties of GaN/AlN quantum dots on Si(111) subject to in-plane uniaxial stresses and variable excitation

NASA Astrophysics Data System (ADS)

Moshe, O.; Rich, D. H.; Birner, S.; Povolotskyi, M.; Damilano, B.; Massies, J.

2010-10-01

We have studied the excitation- and polarization-dependent optical properties of GaN/AlN self-assembled quantum dots (QDs) grown on Si(111) substrates. Ensembles of QDs were subject to various external stress configurations that resulted from the thermal expansion coefficient mismatch between the GaN/AlN layers and the Si(111) substrate and ranged from in-plane uniaxial stress, primarily along the ⟨112¯0⟩ directions, to in-plane biaxial stress, having magnitudes ranging from 20-30 kbar. Limited regions of uniaxial stress were obtained by exploiting naturally occurring microcracks that form during the postgrowth cooling. These microcracks act as stressors in order to create the highly localized regions of uniaxial stress. The local strain tensors for such QDs, which are subject to an interfacial stress perturbation, have been determined by modeling the dependence of the QD excitonic transition energy on the interfacial stress. Cathodoluminescence (CL) measurements of the excitonic transitions exhibit an in-plane linear polarization anisotropy in close proximity to microcracks. The polarization anisotropy is strongly dependent on the sample temperature and the electron beam excitation conditions used to excite the QD ensemble. Localized CL spectroscopy of the QDs exhibits emissions from both the ground and excited states, whose relative contributions depend on the level of excitation and temperature. Experimental results indicate that the polarization anisotropy vanishes at high temperatures (˜300 K) with an increasing excitation of the QDs, while the anisotropy decreases more slowly with excitation at low temperatures (˜60 K). A theoretical modeling of the effect of carrier filling on the polarization anisotropy and the excitonic transition energy was performed, as based on three-dimensional self-consistent solutions of the Schrödinger and Poisson equations using the 6×6 kṡp and effective mass methods for calculations of the e-h wave functions and electron and hole quasi-Fermi levels for varying levels of state filling. We attribute carrier filling and a thermal excitation of holes into higher energy QD hole states during excitation to account for the observed gradual decrease in the polarization anisotropy with an increasing electron-hole pair excitation density at T =300 K.

Influence of VO2+ ions on structural and optical properties of potassium succinate-succinic acid single crystal for non-linear optical applications

NASA Astrophysics Data System (ADS)

Juliet sheela, K.; Subramanian, P.

2018-04-01

A transparent and good optical quality semi organic single crystal of vanadium doped potassium succinate-succinic acid (KSSA) was synthesized by slow evaporation technique at room temperature. The structural perfection was supported by the powder XRD of the KSSA-VO2+ single crystal. Optical behavior of the material was discovered from the absorption and transmission spectra of UV-vis-NIR characterization. Functional group and presence of metal ion in the specimen are depicted from FTIR traces. From the photoluminescence studies, emission of wavelength in the violet region (418 nm) at the excitation of 243 nm could be ascertained. EDAX, SEM measurements identify presence of elements and pictures the step-line growth and the imperfection presents in the grown crystal. EPR analysis extracts the information about the local site symmetry around the impurity ion, molecular orbital coefficients, admixture coefficients and ground state wave function of VO2+ doped KSSA single crystal. Second harmonic generation (SHG) efficiency of the grown crystal was investigated to explore the NLO characteristic of the material.

Optical spectroscopy of excited exciton states in MoS2 monolayers in van der Waals heterostructures

NASA Astrophysics Data System (ADS)

Robert, C.; Semina, M. A.; Cadiz, F.; Manca, M.; Courtade, E.; Taniguchi, T.; Watanabe, K.; Cai, H.; Tongay, S.; Lassagne, B.; Renucci, P.; Amand, T.; Marie, X.; Glazov, M. M.; Urbaszek, B.

2018-01-01

The optical properties of MoS2 monolayers are dominated by excitons, but for spectrally broad optical transitions in monolayers exfoliated directly onto SiO2 substrates detailed information on excited exciton states is inaccessible. Encapsulation in hexagonal boron nitride (hBN) allows approaching the homogenous exciton linewidth, but interferences in the van der Waals heterostructures make direct comparison between transitions in optical spectra with different oscillator strength more challenging. Here we reveal in reflectivity and in photoluminescence excitation spectroscopy the presence of excited states of the A exciton in MoS2 monolayers encapsulated in hBN layers of calibrated thickness, allowing us to extrapolate an exciton binding energy of ≈220 meV. We theoretically reproduce the energy separations and oscillator strengths measured in reflectivity by combining the exciton resonances calculated for a screened two-dimensional Coulomb potential with transfer matrix calculations of the reflectivity for the van der Waals structure. Our analysis shows a very different evolution of the exciton oscillator strength with principal quantum number for the screened Coulomb potential as compared to the ideal two-dimensional hydrogen model.

Reconfigurable visible nanophotonic switch for optogenetic applications (Conference Presentation)

NASA Astrophysics Data System (ADS)

Mohanty, Aseema; Li, Qian; Tadayon, Mohammad Amin; Bhatt, Gaurang R.; Cardenas, Jaime; Miller, Steven A.; Kepecs, Adam; Lipson, Michal

2017-02-01

High spatiotemporal resolution deep-brain optical excitation for optogenetics would enable activation of specific neural populations and in-depth study of neural circuits. Conventionally, a single fiber is used to flood light into a large area of the brain with limited resolution. The scalability of silicon photonics could enable neural excitation over large areas with single-cell resolution similar to electrical probes. However, active control of these optical circuits has yet to be demonstrated for optogenetics. Here we demonstrate the first active integrated optical switch for neural excitation at 473 nm, enabling control of multiple beams for deep-brain neural stimulation. Using a silicon nitride waveguide platform, we develop a cascaded Mach-Zehnder interferometer (MZI) network located outside the brain to direct light to 8 different grating emitters located at the tip of the neural probe. We use integrated platinum microheaters to induce a local thermo-optic phase shift in the MZI to control the switch output. We measure an ON/OFF extinction ratio of >8dB for a single switch and a switching speed of 20 microseconds. We characterize the optical output of the switch by imaging its excitation of fluorescent dye. Finally, we demonstrate in vivo single-neuron optical activation from different grating emitters using a fully packaged device inserted into a mouse brain. Directly activated neurons showed robust spike firing activities with low first-spike latency and small jitter. Active switching on a nanophotonic platform is necessary for eventually controlling highly-multiplexed reconfigurable optical circuits, enabling high-resolution optical stimulation in deep-brain regions.

Nonlinear optical and multiphoton processes for in situ manipulation and conversion of photons: applications to energy and healthcare (Conference Presentation)

NASA Astrophysics Data System (ADS)

Prasad, Paras N.

2017-02-01

Chiral control of nonlinear optical functions holds a great promise for a wide range of applications including optical signal processing, bio-sensing and chiral bio-imaging. In chiral polyfluorene thin films, we demonstrated extremely large chiral nonlinearity. The physics of manipulating excitation dynamics for photon transformation will be discussed, along with nanochemistry control of upconversion in hierarchically built organic chromophore coupled-core-multiple shell nanostructures which enable introduce new, organic-inorganic energy transfer routes for broadband light harvesting and increased upconversion efficiency via multistep cascaded energy transfer. We are pursuing the applications of photon conversion technology in IR harvesting for photovoltaics, high contrast bioimaging, photoacoustic imaging, photodynamic therapy, and optogenetics. An important application is in Brain research and Neurophotonics for functional mapping and modulation of brain activities. Another new direction pursued is magnetic field control of light in in a chiral polymer nanocomposite to achieve large magneto-optic coefficient which can enable sensing of extremely weak magnetic field due to brain waves. Finally, we will consider the thought provoking concept of utilizing photons to quantify, through magneto-optics, and augment - through nanoptogenetics, the cognitive states, thus paving the path way to a quantified human paradigm.

Donor impurity-related linear and nonlinear intraband optical absorption coefficients in quantum ring: effects of applied electric field and hydrostatic pressure

PubMed Central

2012-01-01

The linear and nonlinear intraband optical absorption coefficients in GaAs three-dimensional single quantum rings are investigated. Taking into account the combined effects of hydrostatic pressure and electric field, applied along the growth direction of the heterostructure, the energies of the ground and first excited states of a donor impurity have been found using the effective mass approximation and a variational method. The energies of these states are examined as functions of the dimensions of the structure, electric field, and hydrostatic pressure. We have also investigated the dependencies of the linear, nonlinear, and total optical absorption coefficients as a function of incident photon energy for several configurations of the system. It is found that the variation of distinct sizes of the structure leads to either a redshift and/or a blueshift of the resonant peaks of the intraband optical spectrum. In addition, we have found that the application of an electric field leads to a redshift, whereas the influence of hydrostatic pressure leads to a blueshift (in the case of on-ring-center donor impurity position) of the resonant peaks of the intraband optical spectrum. PMID:23021497

Strong anisotropic optical conductivity in two-dimensional puckered structures: The role of the Rashba effect

NASA Astrophysics Data System (ADS)

Saberi-Pouya, S.; Vazifehshenas, T.; Salavati-fard, T.; Farmanbar, M.; Peeters, F. M.

2017-08-01

We calculate the optical conductivity of an anisotropic two-dimensional system with Rashba spin-flip excitation within the Kubo formalism. We show that the anisotropic Rashba effect caused by an external field significantly changes the magnitude of the spin splitting. Furthermore, we obtain an analytical expression for the longitudinal optical conductivity associated with interband transitions as a function of the frequency for arbitrary polarization angle. We find that the diagonal components of the optical conductivity tensor are direction dependent and the optical absorption spectrum exhibits a strongly anisotropic absorption window. The height and width of this absorption window are very sensitive to the anisotropy of the system. While the height of absorption peak increases with increasing effective mass anisotropy ratio, the peak intensity is larger when the light polarization is along the armchair direction. Moreover, the absorption peak width becomes broader as the density-of-states mass or Rashba interaction is enhanced. These features in the optical absorption spectrum can be used to determine parameters relevant for spintronics.

Optical workstation with concurrent, independent multiphoton imaging and experimental laser microbeam capabilities

PubMed Central

Wokosin, David L.; Squirrell, Jayne M.; Eliceiri, Kevin W.; White, John G.

2008-01-01

Experimental laser microbeam techniques have become established tools for studying living specimens. A steerable, focused laser beam may be used for a variety of experimental manipulations such as laser microsurgery, optical trapping, localized photolysis of caged bioactive probes, and patterned photobleaching. Typically, purpose-designed experimental systems have been constructed for each of these applications. In order to assess the consequences of such experimental optical interventions, long-term, microscopic observation of the specimen is often required. Multiphoton excitation, because of its ability to obtain high-contrast images from deep within a specimen with minimal phototoxic effects, is a preferred technique for in vivo imaging. An optical workstation is described that combines the functionality of an experimental optical microbeam apparatus with a sensitive multiphoton imaging system designed for use with living specimens. Design considerations are discussed and examples of ongoing biological applications are presented. The integrated optical workstation concept offers advantages in terms of flexibility and versatility relative to systems implemented with separate imaging and experimental components. PMID:18607511

Optical workstation with concurrent, independent multiphoton imaging and experimental laser microbeam capabilities

NASA Astrophysics Data System (ADS)

Wokosin, David L.; Squirrell, Jayne M.; Eliceiri, Kevin W.; White, John G.

2003-01-01

Experimental laser microbeam techniques have become established tools for studying living specimens. A steerable, focused laser beam may be used for a variety of experimental manipulations such as laser microsurgery, optical trapping, localized photolysis of caged bioactive probes, and patterned photobleaching. Typically, purpose-designed experimental systems have been constructed for each of these applications. In order to assess the consequences of such experimental optical interventions, long-term, microscopic observation of the specimen is often required. Multiphoton excitation, because of its ability to obtain high-contrast images from deep within a specimen with minimal phototoxic effects, is a preferred technique for in vivo imaging. An optical workstation is described that combines the functionality of an experimental optical microbeam apparatus with a sensitive multiphoton imaging system designed for use with living specimens. Design considerations are discussed and examples of ongoing biological applications are presented. The integrated optical workstation concept offers advantages in terms of flexibility and versatility relative to systems implemented with separate imaging and experimental components.

Multi-Modal Nano-Probes for Radionuclide and 5-color Near Infrared Optical Lymphatic Imaging

PubMed Central

Kobayashi, Hisataka; Koyama, Yoshinori; Barrett, Tristan; Hama, Yukihiro; Regino, Celeste A. S.; Shin, In Soo; Jang, Beom-Su; Le, Nhat; Paik, Chang H.; Choyke, Peter L.; Urano, Yasuteru

2008-01-01

Current contrast agents generally have one function and can only be imaged in monochrome, therefore, the majority of imaging methods can only impart uniparametric information. A single nano-particle has the potential to be loaded with multiple payloads. Such multi-modality probes have the ability to be imaged by more than one imaging technique, which could compensate for the weakness or even combine the advantages of each individual modality. Furthermore, optical imaging using different optical probes enables us to achieve multi-color in vivo imaging, wherein multiple parameters can be read from a single image. To allow differentiation of multiple optical signals in vivo, each probe should have a close but different near infrared emission. To this end, we synthesized nano-probes with multi-modal and multi-color potential, which employed a polyamidoamine dendrimer platform linked to both radionuclides and optical probes, permitting dual-modality scintigraphic and 5-color near infrared optical lymphatic imaging using a multiple excitation spectrally-resolved fluorescence imaging technique. PMID:19079788

Multimodal nanoprobes for radionuclide and five-color near-infrared optical lymphatic imaging.

PubMed

Kobayashi, Hisataka; Koyama, Yoshinori; Barrett, Tristan; Hama, Yukihiro; Regino, Celeste A S; Shin, In Soo; Jang, Beom-Su; Le, Nhat; Paik, Chang H; Choyke, Peter L; Urano, Yasuteru

2007-11-01

Current contrast agents generally have one function and can only be imaged in monochrome; therefore, the majority of imaging methods can only impart uniparametric information. A single nanoparticle has the potential to be loaded with multiple payloads. Such multimodality probes have the ability to be imaged by more than one imaging technique, which could compensate for the weakness or even combine the advantages of each individual modality. Furthermore, optical imaging using different optical probes enables us to achieve multicolor in vivo imaging, wherein multiple parameters can be read from a single image. To allow differentiation of multiple optical signals in vivo, each probe should have a close but different near-infrared emission. To this end, we synthesized nanoprobes with multimodal and multicolor potential, which employed a polyamidoamine dendrimer platform linked to both radionuclides and optical probes, permitting dual-modality scintigraphic and five-color near-infrared optical lymphatic imaging using a multiple-excitation spectrally resolved fluorescence imaging technique.

Luminescent single-walled carbon nanotube-sensitized europium nanoprobes for cellular imaging

PubMed Central

Avti, Pramod K; Sitharaman, Balaji

2012-01-01

Lanthanoid-based optical probes with excitation wavelengths in the ultra-violet (UV) range (300–325 nm) have been widely developed as imaging probes. Efficient cellular imaging requires that lanthanoid optical probes be excited at visible wavelengths, to avoid UV damage to cells. The efficacy of europium-catalyzed single-walled carbon nanotubes (Eu-SWCNTs), as visible nanoprobes for cellular imaging, is reported in this study. Confocal fluorescence microscopy images of breast cancer cells (SK-BR-3 and MCF-7) and normal cells (NIH 3T3), treated with Eu-SWCNT at 0.2 μg/mL concentration, showed bright red luminescence after excitation at 365 nm and 458 nm wavelengths. Cell viability analysis showed no cytotoxic effects after the incubation of cells with Eu-SWCNTs at this concentration. Eu-SWCNT uptake is via the endocytosis mechanism. Labeling efficiency, defined as the percentage of incubated cells that uptake Eu-SWCNT, was 95%–100% for all cell types. The average cellular uptake concentration was 6.68 ng Eu per cell. Intracellular localization was further corroborated by transmission electron microscopy and Raman microscopy. The results indicate that Eu-SWCNT shows potential as a novel cellular imaging probe, wherein SWCNT sensitizes Eu3+ ions to allow excitation at visible wavelengths, and stable time-resolved red emission. The ability to functionalize biomolecules on the exterior surface of Eu-SWCNT makes it an excellent candidate for targeted cellular imaging. PMID:22619533

An affordable optically stimulated luminescent dosimeter reader utilizing multiple excitation wavelengths.

PubMed

Kearfott, Kimberlee J; West, W Geoffrey

2015-10-01

A lower-cost optically stimulated luminescence (OSL) reader with increased flexibility for pursuing laboratory research into OSL theory and application was designed and constructed. This was achieved by using off-the-shelf optical components and higher-power light emitting diodes. The resulting reader includes more wavelengths of excitation light than current commercial readers, as well as the ability to swap out filters and other components during an experiment. Copyright © 2015 Elsevier Ltd. All rights reserved.

Polarization-dependent force driving the Eg mode in bismuth under optical excitation: comparison of first-principles theory with ultra-fast x-ray experiments

NASA Astrophysics Data System (ADS)

Fahy, Stephen; Murray, Eamonn

2015-03-01

Using first principles electronic structure methods, we calculate the induced force on the Eg (zone centre transverse optical) phonon mode in bismuth immediately after absorption of a ultrafast pulse of polarized light. To compare the results with recent ultra-fast, time-resolved x-ray diffraction experiments, we include the decay of the force due to carrier scattering, as measured in optical Raman scattering experiments, and simulate the optical absorption process, depth-dependent atomic driving forces, and x-ray diffraction in the experimental geometry. We find excellent agreement between the theoretical predictions and the observed oscillations of the x-ray diffraction signal, indicating that first-principles theory of optical absorption is well suited to the calculation of initial atomic driving forces in photo-excited materials following ultrafast excitation. This work is supported by Science Foundation Ireland (Grant No. 12/IA/1601) and EU Commission under the Marie Curie Incoming International Fellowships (Grant No. PIIF-GA-2012-329695).

Manipulation of resonant Auger processes with strong optical fields

NASA Astrophysics Data System (ADS)

Picón, Antonio; Buth, Christian; Doumy, Gilles; Krässig, Bertold; Young, Linda; Southworth, Stephen

2013-05-01

We recently reported on the optical control of core-excited states of a resonant Auger process in neon. We have focused on the resonant excitation 1 s --> 1s-1 3 p , while a strong optical field may resonantly couple two core-excited states (1s-1 3 p and 1s-1 3 s) in the Rydberg manifold as well as dressing the continuum. There is a clear signature in the Auger electron spectrum of the inner-shell dynamics induced by the strong optical field: i) the Auger electron spectrum is modified by the rapid optical-induced population transfer from the 1s-1 3 p state to the 1s-1 3 s state during their decay. ii) The angular anisotropy parameter, defining the angular distribution of the Auger electron, is manifested in the envelope of the (angle-integrated) sidebands. This work is funded by the Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy, under Contract No. DE-AC02-06CH11357.

Light Sheet Fluorescence Microscopy (LSFM)

PubMed Central

Adams, Michael W.; Loftus, Andrew F.; Dunn, Sarah E.; Joens, Matthew S.; Fitzpatrick, James A.J.

2015-01-01

The development of confocal microscopy techniques introduced the ability to optically section fluorescent samples in the axial dimension, perpendicular to the image plane. These approaches, via the placement of a pinhole in the conjugate image plane, provided superior resolution in the axial (z) dimension resulting in nearly isotropic optical sections. However, increased axial resolution, via pinhole optics, comes at the cost of both speed and excitation efficiency. Light Sheet Fluorescent Microscopy (LSFM), a century old idea (Siedentopf and Zsigmondy, 1902) made possible with modern developments in both excitation and detection optics, provides sub-cellular resolution and optical sectioning capabilities without compromising speed or excitation efficiency. Over the past decade, several variations of LSFM have been implemented each with its own benefits and deficiencies. Here we discuss LSFM fundamentals and outline the basic principles of several major light sheet based imaging modalities (SPIM, inverted SPIM, multi-view SPIM, Bessel beam SPIM, and stimulated emission depletion SPIM while considering their biological relevance in terms of intrusiveness, temporal resolution, and sample requirements. PMID:25559221

Optical Control of Mechanical Mode-Coupling within a MoS2 Resonator in the Strong-Coupling Regime.

PubMed

Liu, Chang-Hua; Kim, In Soo; Lauhon, Lincoln J

2015-10-14

Two-dimensional (2-D) materials including graphene and transition metal dichalcogenides (TMDs) are an exciting platform for ultrasensitive force and displacement detection in which the strong light-matter coupling is exploited in the optical control of nanomechanical motion. Here we report the optical excitation and displacement detection of a ∼ 3 nm thick MoS2 resonator in the strong-coupling regime, which has not previously been achieved in 2-D materials. Mechanical mode frequencies can be tuned by more than 12% by optical heating, and they exhibit avoided crossings indicative of strong intermode coupling. When the membrane is optically excited at the frequency difference between vibrational modes, normal mode splitting is observed, and the intermode energy exchange rate exceeds the mode decay rate by a factor of 15. Finite element and analytical modeling quantifies the extent of mode softening necessary to control intermode energy exchange in the strong coupling regime.

Thermal stability, optical and Photoluminescence properties of spherical Ce x Zr1‑x O2 (x = 0.05) crystalline blue-emitting nanophosphors synthesized by microwave method

NASA Astrophysics Data System (ADS)

Manjunatha, S.; Dharmaprakash, M. S.

2018-03-01

Nanocrystalline ZrO2 based material is an impressive candidate for the various functional applications owing to their ease of preparation and high thermal stability. This paper reports the synthesis, structural and optical characterization of thermally stable monodispersed CexZr1‑xO2 (x = 0.05) nanoparticles. This method is based on the fact that, microwave irradiation allows the formation of size controlled and single phase cubic ZrO2 nanoparticles containing Ce+4 as a dopant. The XRD and Rietveld analysis revealed the formation of the crystalline cubic fluorite phase. The formation of nanoparticles was confirmed by FTIR. The morphology of the nanophosphors was characterised by FESEM and TEM. The optical band gap was calculated from the UV–visible absorption spectra and was found to vary from 3.93 to 4.25 eV with calcination temperature. It shows the decrease in the optical band gap from the pristine ZrO2. The particle size was measured by using HRTEM, and the average particle size was found to be 22 nm. Under the 268 nm Ultra Violet irradiation excitation a blue emission at 443 nm was observed at room temperature. The possible luminescence mechanism of CexZr1‑xO2 nanophosphor under UV excitation is discussed.

Elastic and inelastic scattering of alpha particles on /sup 5/8Ni and /sup 6/0Ni in a broad range of energy and angle

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

Budzanowski, A.; Dabrowski, H.; Freindl, L.

1978-03-01

The differential cross sections for ..cap alpha.. particles elastically and inelastically scattered from /sup 5/8Ni (at 29, 34, 38, and 58 MeV) and elastically scattered from /sup 6/0Ni (at 29 and 34 MeV), are measured together with excitation functions in the 25--38 MeV region at 178.5/sup 0/ lab. These data together with the data of 26.5, 32.3, 104, and 139 MEV for /sup 5/8Ni and 32.3 and 104 MeV for /sup 6/0Ni from other sources were analyzed using an optical model with volume and surface absorptions and the Saxon-Woods square form factors. The analysis yielded energy dependent depths of bothmore » real and imaginary parts of the potential and constant geometric parameters. The analytical expressions for depths of the real and both absorption potentials are obtained. The coupled channel calculations using the above optical potential were performed for the first excited state of /sup 5/8Ni. Both elastic scattering data and coupling with the first excited state of /sup 5/8Ni are well reproduced using the above potential in the wide scattering energy range.« less

Pressure Dependence of Excitation Cross Sections for Resonant Levels of Rare Gases

NASA Astrophysics Data System (ADS)

Stewart, Michael D.; Chilton, J. Ethan; Lin, Chun C.

2000-06-01

In the rare gases, the excited n'p^5ns and n'p^5nd levels with J = 1 are optically coupled to ground as well as lower lying p levels. Resonant photons emitted when the atom decays to ground can be reabsorbed by another ground-state atom. At low gas pressures this reabsorption occurs infrequently, but at higher pressures becomes increasingly likely until the resonant transition is completely suppressed. This enhances the cascade transitions into lower p levels, resulting in pressure dependent optical emission cross sections. This reabsorption process can be understood quantitatively with a model developed by Heddle et al(D. W. O. Heddle and N. J. Samuel, J. Phys. B 3), 1593 (1970).. The radiation from transitions into the nonresonant levels often lie in the ir, while the resonant radiation is always in the uv spectral region. Using a Fourier-transform spectrometer, one can measure the cross sections for the ir transitions as a function of pressure. The Heddle model can be fit to these data with the use of theoretical values for the Einstein A coefficients. This provides a test of the accuracy of calculated A values. Discussion will include cross section measurements for Ne, Ar, and Kr excited by electron impact over a range of gas pressures.

Towards two-photon excited endogenous fluorescence lifetime imaging microendoscopy

PubMed Central

Hage, C. H.; Leclerc, P.; Brevier, J.; Fabert, M.; Le Nézet, C.; Kudlinski, A.; Héliot, L.; Louradour, F.

2017-01-01

In situ fluorescence lifetime imaging microscopy (FLIM) in an endoscopic configuration of the endogenous biomarker nicotinamide adenine dinucleotide (NADH) has a great potential for malignant tissue diagnosis. Moreover, two-photon nonlinear excitation provides intrinsic optical sectioning along with enhanced imaging depth. We demonstrate, for the first time to our knowledge, nonlinear endogenous FLIM in a fibered microscope with proximal detection, applied to NADH in cultured cells, as a first step to a nonlinear endomicroscope, using a double-clad microstructured fiber with convenient fiber length (> 3 m) and excitation pulse duration (≈50 fs). Fluorescence photons are collected by the fiber inner cladding and we show that its contribution to the impulse response function (IRF), which originates from its intermodal and chromatic dispersions, is small (< 600 ps) and stable for lengths up to 8 m and allows for short lifetime measurements. We use the phasor representation as a quick visualization tool adapted to the endoscopy speed requirements. PMID:29359093

Capillary waveguide optrodes: an approach to optical sensing in medical diagnostics

NASA Astrophysics Data System (ADS)

Lippitsch, Max E.; Draxler, Sonja; Kieslinger, Dietmar; Lehmann, Hartmut; Weigl, Bernhard H.

1996-07-01

Glass capillaries with a chemically sensitive coating on the inner surface are used as optical sensors for medical diagnostics. A capillary simultaneously serves as a sample compartment, a sensor element, and an inhomogeneous optical waveguide. Various detection schemes based on absorption, fluorescence intensity, or fluorescence lifetime are described. In absorption-based capillary waveguide optrodes the absorption in the sensor layer is analyte dependent; hence light transmission along the inhomogeneous waveguiding structure formed by the capillary wall and the sensing layer is a function of the analyte concentration. Similarly, in fluorescence-based capillary optrodes the fluorescence intensity or the fluorescence lifetime of an indicator dye fixed in the sensing layer is analyte dependent; thus the specific property of fluorescent light excited in the sensing layer and thereafter guided along the inhomogeneous waveguiding structure is a function of the analyte concentration. Both schemes are experimentally demonstrated, one with carbon dioxide as the analyte and the other one with oxygen. The device combines optical sensors with the standard glass capillaries usually applied to gather blood drops from fingertips, to yield a versatile diagnostic instrument, integrating the sample compartment, the optical sensor, and the light-collecting optics into a single piece. This ensures enhanced sensor performance as well as improved handling compared with other sensors. waveguide, blood gases, medical diagnostics.

Porous silicon-VO{sub 2} based hybrids as possible optical temperature sensor: Wavelength-dependent optical switching from visible to near-infrared range

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

Antunez, E. E.; Salazar-Kuri, U.; Estevez, J. O.

Morphological properties of thermochromic VO{sub 2}—porous silicon based hybrids reveal the growth of well-crystalized nanometer-scale features of VO{sub 2} as compared with typical submicron granular structure obtained in thin films deposited on flat substrates. Structural characterization performed as a function of temperature via grazing incidence X-ray diffraction and micro-Raman demonstrate reversible semiconductor-metal transition of the hybrid, changing from a low-temperature monoclinic VO{sub 2}(M) to a high-temperature tetragonal rutile VO{sub 2}(R) crystalline structure, coupled with a decrease in phase transition temperature. Effective optical response studied in terms of red/blue shift of the reflectance spectra results in a wavelength-dependent optical switching withmore » temperature. As compared to VO{sub 2} film over crystalline silicon substrate, the hybrid structure is found to demonstrate up to 3-fold increase in the change of reflectivity with temperature, an enlarged hysteresis loop and a wider operational window for its potential application as an optical temperature sensor. Such silicon based hybrids represent an exciting class of functional materials to display thermally triggered optical switching culminated by the characteristics of each of the constituent blocks as well as device compatibility with standard integrated circuit technology.« less

Coupling Light Emitting Diodes with Photocatalyst-Coated Optical Fibers Improves Quantum Yield of Pollutant Oxidation.

PubMed

Ling, Li; Tugaoen, Heather; Brame, Jonathon; Sinha, Shahnawaz; Li, Chuanhao; Schoepf, Jared; Hristovski, Kiril; Kim, Jae-Hong; Shang, Chii; Westerhoff, Paul

2017-11-21

A photocatalyst-coated optical fiber was coupled with a 318 nm ultraviolet-A light emitting diode, which activated the photocatalysts by interfacial photon-electron excitation while minimizing photonic energy losses due to conventional photocatalytic barriers. The light delivery mechanism was explored via modeling of evanescent wave energy produced upon total internal reflection and photon refraction into the TiO 2 surface coating. This work explores aqueous phase LED-irradiated optical fibers for treating organic pollutants and for the first time proposes a dual-mechanistic approach to light delivery and photocatalytic performance. Degradation of a probe organic pollutant was evaluated as a function of optical fiber coating thickness, fiber length, and photocatalyst attachment method and compared against the performance of an equivalent catalyst mass in a completely mixed slurry reactor. Measured and simulated photon fluence through the optical fibers decreased as a function of fiber length, coating thickness, or TiO 2 mass externally coated on the fiber. Thinner TiO 2 coatings achieved faster pollutant removal rates from solution, and dip coating performed better than sol-gel attachment methods. TiO 2 attached to optical fibers achieved a 5-fold higher quantum yield compared against an equivalent mass of TiO 2 suspended in a slurry solution.

Electrodeless-discharge-vapor-lamp-based Faraday anomalous-dispersion optical filter.

PubMed

Sun, Qinqing; Zhuang, Wei; Liu, Zhiwen; Chen, Jingbiao

2011-12-01

We report an excited-state Faraday anomalous-dispersion optical filter operating on the rubidium 5P(3/2)-5D(5/2) transition (775.9 nm in vacuum) without the use of a pump laser. An electrodeless discharge vapor lamp is employed to replace the Rb vapor cell in a traditional Faraday anomalous-dispersion optical filter system. Atoms can be excited by power rather than a complex frequency-locked pump laser. A proof-of-concept experimental demonstration with a maximum transmission of 1.9% and a filter bandwidth of 650 MHz is presented. © 2011 Optical Society of America

Picosecond Transient Photoconductivity in Functionalized Pentacene Molecular Crystals Probed by Terahertz Pulse Spectroscopy

NASA Astrophysics Data System (ADS)

Hegmann, F. A.; Tykwinski, R. R.; Lui, K. P.; Bullock, J. E.; Anthony, J. E.

2002-11-01

We have measured transient photoconductivity in functionalized pentacene molecular crystals using ultrafast optical pump-terahertz probe techniques. The single crystal samples were excited using 800nm, 100fs pulses, and the change in transmission of time-delayed, subpicosecond terahertz pulses was used to probe the photoconducting state over a temperature range from 10 to 300K. A subpicosecond rise in photoconductivity is observed, suggesting that mobile carriers are a primary photoexcitation. At times longer than 4ps, a power-law decay is observed consistent with dispersive transport.

A five-primary photostimulator suitable for studying intrinsically photosensitive retinal ganglion cell functions in humans

PubMed Central

Cao, Dingcai; Nicandro, Nathaniel; Barrionuevo, Pablo A.

2015-01-01

Intrinsically photosensitive retinal ganglion cells (ipRGCs) can respond to light directly through self-contained photopigment, melanopsin. IpRGCs also receive synaptic inputs from rods and cones. Thus, studying ipRGC functions requires a novel photostimulating method that can account for all of the photoreceptor inputs. Here, we introduced an inexpensive LED-based five-primary photostimulator that can control the excitations of rods, S-, M-, L-cones, and melanopsin-containing ipRGCs in humans at constant background photoreceptor excitation levels, a critical requirement for studying the adaptation behavior of ipRGCs with rod, cone, or melanopsin input. We described the theory and technical aspects (including optics, electronics, software, and calibration) of the five-primary photostimulator. Then we presented two preliminary studies using the photostimulator we have implemented to measure melanopsin-mediated pupil responses and temporal contrast sensitivity function (TCSF). The results showed that the S-cone input to pupil responses was antagonistic to the L-, M- or melanopsin inputs, consistent with an S-OFF and (L + M)-ON response property of primate ipRGCs (Dacey et al., 2005). In addition, the melanopsin-mediated TCSF had a distinctive pattern compared with L + M or S-cone mediated TCSF. Other than controlling individual photoreceptor excitation independently, the five-primary photostimulator has the flexibility in presenting stimuli modulating any combination of photoreceptor excitations, which allows researchers to study the mechanisms by which ipRGCs combine various photoreceptor inputs. PMID:25624466

Bend-insensitive distributed sensing in singlemode-multimode-singlemode optical fiber structure by using Brillouin optical time-domain analysis.

PubMed

Xu, Pengbai; Dong, Yongkang; Zhang, Juwang; Zhou, Dengwang; Jiang, Taofei; Xu, Jinlong; Zhang, Hongying; Zhu, Tao; Lu, Zhiwei; Chen, Liang; Bao, Xiaoyi

2015-08-24

We propose a bend-insensitive distributed Brillouin optical fiber sensing by using a singlemode-multimode-singlemode optical fiber structure for the first time to the best of our knowledge. The sensing fiber is a graded-index multimode fiber (GI-MMF) sandwiched by two standard single-mode fibers (SMFs) with central-alignment splicing at the interface between GI-MMF and SMF to excite the fundamental mode in GI-MMF. The sensing system can resist a minimal bend radius of 1.25mm while maintain the measurement performance, with which the measured coefficients of strain and temperature are 421.6MHz/% and 0.826MHz/°C, respectively. We also demonstrate that the higher-order modes excited in GI-MMF can be easily influenced by bending, so that exciting the fundamental mode is essential for bend-insensitive distributed sensing.

Coherent Spin Control at the Quantum Level in an Ensemble-Based Optical Memory.

PubMed

Jobez, Pierre; Laplane, Cyril; Timoney, Nuala; Gisin, Nicolas; Ferrier, Alban; Goldner, Philippe; Afzelius, Mikael

2015-06-12

Long-lived quantum memories are essential components of a long-standing goal of remote distribution of entanglement in quantum networks. These can be realized by storing the quantum states of light as single-spin excitations in atomic ensembles. However, spin states are often subjected to different dephasing processes that limit the storage time, which in principle could be overcome using spin-echo techniques. Theoretical studies suggest this to be challenging due to unavoidable spontaneous emission noise in ensemble-based quantum memories. Here, we demonstrate spin-echo manipulation of a mean spin excitation of 1 in a large solid-state ensemble, generated through storage of a weak optical pulse. After a storage time of about 1 ms we optically read-out the spin excitation with a high signal-to-noise ratio. Our results pave the way for long-duration optical quantum storage using spin-echo techniques for any ensemble-based memory.

Imaging B. anthracis heme catabolism in mice using the IFP1.4 gene reporter

NASA Astrophysics Data System (ADS)

Zhu, Banghe; Robinson, Holly; Wilganowski, Nathaniel; Nobles, Christopher L.; Sevick-Muraca, Eva; Maresso, Anthony

2012-03-01

B. anthracis is a gram-positive, spore-forming bacterium which likes all pathogenic bacteria, survive by sequestering heme from its host. To image B. anthracis heme catabolism in vivo, we stably transfect new red excitable fluorescent protein, IFP1.4, that requires the heme catabolism product biliverdin (BV). IFP1.4 reporter has favorable excitation and emission characteristics, which has an absorption peak at 685 nm and an emission peak at 708 nm. Therefore, IFP1.4 reporter can be imaged deeply into the tissue with less contamination from tissue autofluorescence. However, the excitation light "leakage" through optical filters can limit detection and sensitivity of IFP1.4 reporter due to the small Stoke's shift of IFP1.4 fluorescence. To minimize the excitation light leakage, an intensified CCD (ICCD) based infrared fluorescence imaging device was optimized using two band pass filters separated by a focus lens to increase the optical density at the excitation wavelength. In this study, a mouse model (DBA/J2) was first injected with B. anthracis bacteria expressing IFP1.4, 150 μl s.c., on the ventral side of the left thigh. Then mouse was given 250 μl of a 1mM BV solution via I.V. injection. Imaging was conducted as a function of time after infection under light euthanasia, excised tissues were imaged and IFP1.4 fluorescence correlated with standard culture measurements of colony forming units (CFU). The work demonstrates the use of IFP1.4 as a reporter of bacterial utilization of host heme and may provide an important tool for understanding the pathogenesis of bacterial infection and developing new anti-bacterial therapeutics.

Inversion of the resonance line of Sr/+/ produced by optically pumping Sr atoms

NASA Technical Reports Server (NTRS)

Green, W. R.; Falcone, R. W.

1978-01-01

A description is presented of an experiment which demonstrates the selective production of excited-state ions by an optical absorption from neutrals. An inversion on the resonance line of Sr(+) was produced by laser excitation of a two-electron transition, followed by ionization of one of the excited electrons by the same laser. A pulsed, mode-locked laser operating at 2680 A was used to excite atoms from the Sr ground level. The same laser then ionized the excited atoms. The 2680-A pump beam was generated by frequency doubling the output of a synchronously pumped mode-locked dye laser in a KDP crystal. It is pointed out that the reported results are significant for the construction of vacuum-ultraviolet and X-ray lasers. Many of the proposed methods for making such lasers depend on the selective production of excited-state ions.

A transform from absorption to Raman excitation profile. A time-dependent approach

NASA Astrophysics Data System (ADS)

Lee, Soo-Y.; Yeo, Robert C. K.

1994-04-01

An alternative time-frame approach, which is canonically conjugate to the energy-frame approach, for implementing the transform relations for calculating Raman excitation profiles directly from the optical absorption spectrum is presented. Practical and efficient fast Fourier transformation in the time frame replaces the widely used Chan and Page algorithm for evaluating the Hilbert transform in the energy frame. The time-frame approach is applied to: (a) a two-mode model which illustrates the missing mode effect in both absorption and Raman excitation profiles, (b) carotene, in which both the absorption spectrum and the Raman excitation profile show vibrational structure and (c) hexamethylbenzene: TCNE electron donor—acceptor complex where the same spectra are structureless and the Raman excitation profile for the 168 cm -1 mode poses a problem for the energy-frame approach. A similar time-frame approach can be used for the inverse transform from the Raman excitation profile to the optical absorption spectrum.

Fluorescence-tunable Ag-DNA biosensor with tailored cytotoxicity for live-cell applications

NASA Astrophysics Data System (ADS)

Bossert, Nelli; de Bruin, Donny; Götz, Maria; Bouwmeester, Dirk; Heinrich, Doris

2016-11-01

DNA-stabilized silver clusters (Ag-DNA) show excellent promise as a multi-functional nanoagent for molecular investigations in living cells. The unique properties of these fluorescent nanomaterials allow for intracellular optical sensors with tunable cytotoxicity based on simple modifications of the DNA sequences. Three Ag-DNA nanoagent designs are investigated, exhibiting optical responses to the intracellular environments and sensing-capability of ions, functional inside living cells. Their sequence-dependent fluorescence responses inside living cells include (1) a strong splitting of the fluorescence peak for a DNA hairpin construct, (2) an excitation and emission shift of up to 120 nm for a single-stranded DNA construct, and (3) a sequence robust in fluorescence properties. Additionally, the cytotoxicity of these Ag-DNA constructs is tunable, ranging from highly cytotoxic to biocompatible Ag-DNA, independent of their optical sensing capability. Thus, Ag-DNA represents a versatile live-cell nanoagent addressable towards anti-cancer, patient-specific and anti-bacterial applications.

Two-color single-photon emission from InAs quantum dots: toward logic information management using quantum light.

PubMed

Rivas, David; Muñoz-Matutano, Guillermo; Canet-Ferrer, Josep; García-Calzada, Raúl; Trevisi, Giovanna; Seravalli, Luca; Frigeri, Paola; Martínez-Pastor, Juan P

2014-02-12

In this work, we propose the use of the Hanbury-Brown and Twiss interferometric technique and a switchable two-color excitation method for evaluating the exciton and noncorrelated electron-hole dynamics associated with single photon emission from indium arsenide (InAs) self-assembled quantum dots (QDs). Using a microstate master equation model we demonstrate that our single QDs are described by nonlinear exciton dynamics. The simultaneous detection of two-color, single photon emission from InAs QDs using these nonlinear dynamics was used to design a NOT AND logic transference function. This computational functionality combines the advantages of working with light/photons as input/output device parameters (all-optical system) and that of a nanodevice (QD size of ∼ 20 nm) while also providing high optical sensitivity (ultralow optical power operational requirements). These system features represent an important and interesting step toward the development of new prototypes for the incoming quantum information technologies.

Pharmacological studies upon neurones of the lateral geniculate nucleus of the cat

PubMed Central

Curtis, D. R.; Davis, R.

1962-01-01

Indoles related to 5-hydroxytryptamine, lysergic acid derivatives, phenethylamine derivatives and some other compounds have been applied electrophoretically to the neurones of the lateral geniculate nucleus of the cat anaesthetized with pentobarbitone sodium. Many of these compounds, particularly 4-, 5- and 7-hydroxytryptamine and ergometrine, depress the orthodromic excitation of the neurones by volleys in optic nerve fibres, but do not affect antidromic excitation by volleys in the optic radiation or chemical excitation by L-glutamic acid. It is concluded that the active depressants either block the access of the excitatory transmitter to subsynaptic receptors or prevent the release of the transmitter from optic nerve terminals. The structure-activity relationships of the depressant substances are discussed. PMID:13882768

Limit on Excitation and Stabilization of Atoms in Intense Optical Laser Fields.

PubMed

Zimmermann, H; Meise, S; Khujakulov, A; Magaña, A; Saenz, A; Eichmann, U

2018-03-23

Atomic excitation in strong optical laser fields has been found to take place even at intensities exceeding saturation. The concomitant acceleration of the atom in the focused laser field has been considered a strong link to, if not proof of, the existence of the so-called Kramers-Henneberger (KH) atom, a bound atomic system in an intense laser field. Recent findings have moved the importance of the KH atom from being purely of theoretical interest toward real world applications; for instance, in the context of laser filamentation. Considering this increasing importance, we explore the limits of strong-field excitation in optical fields, which are basically imposed by ionization through the spatial field envelope and the field propagation.

Optical properties of implanted Xe color centers in diamond

DOE PAGES

Sandstrom, Russell; Ke, Li; Martin, Aiden; ...

2017-12-20

Optical properties of color centers in diamond have been the subject of intense research due to their promising applications in quantum photonics. Here in this work we study the optical properties of Xe related color centers implanted into nitrogen rich (type IIA) and an ultrapure, electronic grade diamond. The Xe defect has two zero phonon lines at 794 nm and 811 nm, which can be effectively excited using both green and red excitation, however, its emission in the nitrogen rich diamond is brighter. Near resonant excitation is performed at cryogenic temperatures and luminescence is probed under strong magnetic field. Finally,more » our results are important towards the understanding of the Xe related defect and other near infrared color centers in diamond.« less

Optical properties of implanted Xe color centers in diamond

NASA Astrophysics Data System (ADS)

Sandstrom, Russell; Ke, Li; Martin, Aiden; Wang, Ziyu; Kianinia, Mehran; Green, Ben; Gao, Wei-bo; Aharonovich, Igor

2018-03-01

Optical properties of color centers in diamond have been the subject of intense research due to their promising applications in quantum photonics. In this work we study the optical properties of Xe related color centers implanted into nitrogen rich (type IIA) and an ultrapure, electronic grade diamond. The Xe defect has two zero phonon lines at ∼794 nm and 811 nm, which can be effectively excited using both green and red excitation, however, its emission in the nitrogen rich diamond is brighter. Near resonant excitation is performed at cryogenic temperatures and luminescence is probed under strong magnetic field. Our results are important towards the understanding of the Xe related defect and other near infrared color centers in diamond.

Optical properties of implanted Xe color centers in diamond

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

Sandstrom, Russell; Ke, Li; Martin, Aiden

Optical properties of color centers in diamond have been the subject of intense research due to their promising applications in quantum photonics. Here in this work we study the optical properties of Xe related color centers implanted into nitrogen rich (type IIA) and an ultrapure, electronic grade diamond. The Xe defect has two zero phonon lines at 794 nm and 811 nm, which can be effectively excited using both green and red excitation, however, its emission in the nitrogen rich diamond is brighter. Near resonant excitation is performed at cryogenic temperatures and luminescence is probed under strong magnetic field. Finally,more » our results are important towards the understanding of the Xe related defect and other near infrared color centers in diamond.« less

Study of indium tin oxide films exposed to atomic axygen

NASA Technical Reports Server (NTRS)

Snyder, Paul G.; De, Bhola N.; Woollam, John A.; Coutts, T. J.; Li, X.

1989-01-01

A qualitative simulation of the effects of atomic oxygen has been conducted on indium tin oxide (ITO) films prepared by dc sputtering onto room-temperature substrates, by exposing them to an RF-excited oxygen plasma and characterizing the resulting changes in optical, electrical, and structural properties as functions of exposure time with ellipsometry, spectrophotometry, resistivity, and X-ray measurements. While the films thus exposed exhibit reduced resistivity and optical transmission; both of these effects, as well as partial crystallization of the films, may be due to sample heating by the plasma. Film resistivity is found to stabilize after a period of exposure.

Optical Emission Characterization of High-Power Hall Thruster Wear

NASA Technical Reports Server (NTRS)

WIlliams, George J.; Kamhawi, Hani

2013-01-01

Optical emission spectroscopy is employed to correlate BN insulator erosion with high-power operation of the NASA 300M Hall-effect thruster. Actinometry leveraging excited xenon states is used to normalize the emission spectra of ground state boron as a function of thruster operating condition. Trends in the strength of the boron signal are correlated with thruster power, discharge voltage, discharge current and magnetic field strength. The boron signals are shown to trend with discharge current and show weak dependence on discharge voltage. The trends are consistent with data previously collected on the NASA 300M and NASA 457M thrusters but are different from conventional wisdom.

Thermal conductivity in large - J two-dimensional antiferromagnets: Role of phonon scattering

DOE PAGES

Chernyshev, A. L.; Brenig, Wolfram

2015-08-05

Different types of relaxation processes for magnon heat current are discussed, with a particular focus on coupling to three-dimensional phonons. There is thermal conductivity by these in-plane magnetic excitations using two distinct techniques: Boltzmann formalism within the relaxation-time approximation and memory-function approach. Also considered are the scattering of magnons by both acoustic and optical branches of phonons. We demonstrate an accord between the two methods, regarding the asymptotic behavior of the effective relaxation rates. It is strongly suggested that scattering from optical or zone-boundary phonons is important for magnon heat current relaxation in a high-temperature window of ΘD≲T<< J.

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

Minissale, S.; Yerci, S.; Dal Negro, L.

We investigate the nonlinear optical properties of Si-rich silicon oxide (SRO) and Si-rich silicon nitride (SRN) samples as a function of silicon content, annealing temperature, and excitation wavelength. Using the Z-scan technique, we measure the non-linear refractive index n{sub 2} and the nonlinear absorption coefficient {beta} for a large number of samples fabricated by reactive co-sputtering. Moreover, we characterize the nonlinear optical parameters of SRN in the broad spectral region 1100-1500 nm and show the strongest nonlinearity at 1500 nm. These results demonstrate the potential of the SRN matrix for the engineering of compact devices with enhanced Kerr nonlinearities formore » silicon photonics applications.« less

Effect of temperature on the shape of spatial quasi-periodic oscillations of the refractive index of alkali atoms in an optically dense medium with a closed excitation contour of Δ type

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

Barantsev, K A; Litvinov, A N

2014-10-31

A theory of a closed excitation contour (Δ system) of a three-level atom in an optically dense medium is constructed with allowance for temperature. The spatial quasi-periodic oscillations of the refractive index in the system under study are shown to damp with increasing temperature. The range of temperatures at which these oscillations are most pronounced is found. (quantum optics)

Development of fluorescent tracers for the real-time monitoring of renal function

NASA Astrophysics Data System (ADS)

Poreddy, Amruta R.; Asmelash, Bethel; Debreczeny, Martin P.; Fitch, Richard M.; Freskos, John N.; Galen, Karen P.; Gaston, Kimberly R.; Kostelc, James G.; Kumar, Rana; Marzan, Tim A.; Neumann, William L.; Rajagopalan, Raghavan; Schoenstein, Tasha M.; Shieh, Jeng-Jong; Wilcox, J. Micah; Wojdyla, Jolette K.; Dorshow, Richard B.

2011-03-01

Accurate measurement of glomerular filtration rate (GFR) at the bedside is highly desirable in order to assess renal function in real-time, which is currently an unmet clinical need. In our pursuit to develop exogenous fluorescent tracers as GFR markers, various hydrophilic derivatives of 3,6-diaminopyrazine-2,5-dicarboxylic acid with varying molecular weights and absorption/emission characteristics were synthesized. These include polyhydroxyalkyl based small molecules and poly(ethylene glycol) (PEG) substituted moderate molecular weight compounds, which were further sub-grouped into analogs having blue excitation with green emission, and relatively longer wavelength analogs having green excitation with orange emission. Lead compounds were identified in each of the four classes on the basis of structure- activity relationship studies, which included in vitro plasma protein binding, in vivo urine recovery of administered dose, and in vivo optical monitoring. The in vivo optical monitoring experiments with lead candidates have been correlated with plasma pharmacokinetic (PK) data for measurement of clearance and hence GFR. Renal clearance of these compounds, occurring exclusively via glomerular filtration, was established by probenecid blocking experiments. The renal clearance property of all these advanced candidates was superior to that of the iothalamate, which is currently an accepted standard for the measurement of GFR.

Imaging the Ultrafast Photoelectron Transfer Process in Alizarin-TiO2.

PubMed

Gomez, Tatiana; Hermann, Gunter; Zarate, Ximena; Pérez-Torres, Jhon Fredy; Tremblay, Jean Christophe

2015-07-30

In this work, we adopt a quantum mechanical approach based on time-dependent density functional theory (TDDFT) to study the optical and electronic properties of alizarin supported on TiO2 nano-crystallites, as a prototypical dye-sensitized solar cell. To ensure proper alignment of the donor (alizarin) and acceptor (TiO2 nano-crystallite) levels, static optical excitation spectra are simulated using time-dependent density functional theory in response. The ultrafast photoelectron transfer from the dye to the cluster is simulated using an explicitly time-dependent, one-electron TDDFT ansatz. The model considers the δ-pulse excitation of a single active electron localized in the dye to the complete set of energetically accessible, delocalized molecular orbitals of the dye/nano-crystallite complex. A set of quantum mechanical tools derived from the transition electronic flux density is introduced to visualize and analyze the process in real time. The evolution of the created wave packet subject to absorbing boundary conditions at the borders of the cluster reveal that, while the electrons of the aromatic rings of alizarin are heavily involved in an ultrafast charge redistribution between the carbonyl groups of the dye molecule, they do not contribute positively to the electron injection and, overall, they delay the process.

Microscopy imaging device with advanced imaging properties

DOEpatents

Ghosh, Kunal; Burns, Laurie; El Gamal, Abbas; Schnitzer, Mark J.; Cocker, Eric; Ho, Tatt Wei

2015-11-24

Systems, methods and devices are implemented for microscope imaging solutions. One embodiment of the present disclosure is directed toward an epifluorescence microscope. The microscope includes an image capture circuit including an array of optical sensor. An optical arrangement is configured to direct excitation light of less than about 1 mW to a target object in a field of view of that is at least 0.5 mm.sup.2 and to direct epi-fluorescence emission caused by the excitation light to the array of optical sensors. The optical arrangement and array of optical sensors are each sufficiently close to the target object to provide at least 2.5 .mu.m resolution for an image of the field of view.

Microscopy imaging device with advanced imaging properties

DOEpatents

Ghosh, Kunal; Burns, Laurie; El Gamal, Abbas; Schnitzer, Mark J.; Cocker, Eric; Ho, Tatt Wei

2016-10-25

Systems, methods and devices are implemented for microscope imaging solutions. One embodiment of the present disclosure is directed toward an epifluorescence microscope. The microscope includes an image capture circuit including an array of optical sensor. An optical arrangement is configured to direct excitation light of less than about 1 mW to a target object in a field of view of that is at least 0.5 mm.sup.2 and to direct epi-fluorescence emission caused by the excitation light to the array of optical sensors. The optical arrangement and array of optical sensors are each sufficiently close to the target object to provide at least 2.5 .mu.m resolution for an image of the field of view.

Microscopy imaging device with advanced imaging properties

DOEpatents

Ghosh, Kunal; Burns, Laurie; El Gamal, Abbas; Schnitzer, Mark J.; Cocker, Eric; Ho, Tatt Wei

2016-11-22

Systems, methods and devices are implemented for microscope imaging solutions. One embodiment of the present disclosure is directed toward an epifluorescence microscope. The microscope includes an image capture circuit including an array of optical sensor. An optical arrangement is configured to direct excitation light of less than about 1 mW to a target object in a field of view of that is at least 0.5 mm.sup.2 and to direct epi-fluorescence emission caused by the excitation light to the array of optical sensors. The optical arrangement and array of optical sensors are each sufficiently close to the target object to provide at least 2.5 .mu.m resolution for an image of the field of view.

Microscopy imaging device with advanced imaging properties

DOEpatents

Ghosh, Kunal; Burns, Laurie; El Gamal, Abbas; Schnitzer, Mark J.; Cocker, Eric; Ho, Tatt Wei

2017-04-25

Systems, methods and devices are implemented for microscope imaging solutions. One embodiment of the present disclosure is directed toward an epifluorescence microscope. The microscope includes an image capture circuit including an array of optical sensor. An optical arrangement is configured to direct excitation light of less than about 1 mW to a target object in a field of view of that is at least 0.5 mm.sup.2 and to direct epi-fluorescence emission caused by the excitation light to the array of optical sensors. The optical arrangement and array of optical sensors are each sufficiently close to the target object to provide at least 2.5 .mu.m resolution for an image of the field of view.

Optical spectroscopy of molecular positronium.

PubMed

Cassidy, D B; Hisakado, T H; Tom, H W K; Mills, A P

2012-03-30

We report optical spectroscopic measurements of molecular positronium (Ps(2)), performed via a previously unobserved L=1 excited state. Ps(2) molecules created in a porous silica film, and also in vacuum from an Al(111) crystal, were resonantly excited and then photoionized by pulsed lasers, providing conclusive evidence for the production of this molecular matter-antimatter system and its excited state. Future experiments making use of the photoionized vacuum L=1 Ps(2) could provide a source of Ps(+) ions, as well as other multipositronic systems, such as Ps(2)H(-) or Ps(2)O.

Method and apparatus for imaging a sample on a device

DOEpatents

Trulson, Mark; Stern, David; Fiekowsky, Peter; Rava, Richard; Walton, Ian; Fodor, Stephen P. A.

2001-01-01

A method and apparatus for imaging a sample are provided. An electromagnetic radiation source generates excitation radiation which is sized by excitation optics to a line. The line is directed at a sample resting on a support and excites a plurality of regions on the sample. Collection optics collect response radiation reflected from the sample I and image the reflected radiation. A detector senses the reflected radiation and is positioned to permit discrimination between radiation reflected from a certain focal plane in the sample and certain other planes within the sample.

Quantum Nonlinear Optics without real Photons

NASA Astrophysics Data System (ADS)

Macrí, Vincenzo; Frisk Kockum, Anton; Stassi, Roberto; di Stefano, Omar; Savasta, Salvatore; Nori, Franco

We propose a physical process analogous to spontaneous parametric down-conversion, where one excited atom directly transfers its excitation to a couple of spatially-separated atoms with probability approaching one. The interaction is mediated by the exchange of virtual, rather than real, photons. This nonlinear optical process is coherent and reversible, so that the two excited atoms can transfer back the excitation to the first one: the atomic analogue of sum-frequency generation. The parameters used here correspond to experimentally-demonstrated values in circuit QED. This approach can be extended to consider other nonlinear interatomic processes, e.g. four-qubit mixing, and is an attractive architecture for the realization of quantum devices on a chip. Univ. of Michigan, USA.

Quantum Nonlinear Optics without Photons

NASA Astrophysics Data System (ADS)

Macrı, Vincenzo

Here we propose a physical process analogous to spontaneous parametric down-conversion, where one excited atom directly transfers its excitation to a couple of spatially separated atoms with probability approaching one. The interaction is mediated by the exchange of virtual rather than real photons. This nonlinear optical process is coherent and reversible, so that the couple of excited atoms can transfer back the excitation to the first one: the analogous for atoms of sum-frequency generation. The parameters used here correspond to experimentally-demonstrated values in circuit QED. This approach can be expanded to consider other nonlinear inter-atomic processes as the four-qubit mixing and is an attractive architecture for the realization of quantum devices on a chip.

Experimental results on the ω- and η'-nucleus potential - on the way to mesic states

NASA Astrophysics Data System (ADS)

Nanova, Mariana

2015-06-01

Different experimental approaches to determine the meson-nucleus optical potential are discussed. The experiments have been performed with the Crystal Barrel/TAPS detector system at the ELSA accelerator in Bonn and the Crystal Ball/TAPS at the MAMI accelerator in Mainz. Experimental results about the real and imaginary part of the η'- and ω-nucleus optical potential are presented. The imaginary part of the meson-nucleus optical potential is determined from the in-medium width of the meson by the measurement of the transparency ratio. Information on the real part of the optical potential is deduced from measurements of the excitation function and momentum distribution which are sensitive to the sign and depth of the potential. The results are discussed and compared to theoretical predictions. The data for both mesons are consistent with a weakly attractive potential. The formation and population of ω-nucleus and η'-nucleus bound states is additionally discussed.

Good vibrations: Controlling light with sound (Conference Presentation)

NASA Astrophysics Data System (ADS)

Eggleton, Benjamin J.; Choudhary, Amol

2016-10-01

One of the surprises of nonlinear optics, is that light may interact strongly with sound. Intense laser light literally "shakes" the glass in optical fibres, exciting acoustic waves (sound) in the fibre. Under the right conditions, it leads to a positive feedback loop between light and sound termed "Stimulated Brillouin Scattering," or simply SBS. This nonlinear interaction can amplify or filter light waves with extreme precision in frequency which makes it uniquely suited to solve key problems in the fields of defence, biomedicine, wireless communications, spectroscopy and imaging. We have achieved the first demonstration of SBS in compact chip-scale structures, carefully designed so that the optical fields and the acoustic fields are simultaneously confined and guided. This new platform has opened a range of new functionalities that are being applied in communications and defence with breathtaking performance and compactness. My talk will introduce this new field and review our progress and achievements, including silicon based optical phononic processor.

Fiber optic probe enabled by surface-enhanced Raman scattering for early diagnosis of potential acute rejection of kidney transplant

NASA Astrophysics Data System (ADS)

Chi, Jingmao; Chen, Hui; Tolias, Peter; Du, Henry

2014-06-01

We have explored the use of a fiber-optic probe with surface-enhanced Raman scattering (SERS) sensing modality for early, noninvasive and, rapid diagnosis of potential renal acute rejection (AR) and other renal graft dysfunction of kidney transplant patients. Multimode silica optical fiber immobilized with colloidal Ag nanoparticles at the distal end was used for SERS measurements of as-collected urine samples at 632.8 nm excitation wavelength. All patients with abnormal renal graft function (3 AR episodes and 2 graft failure episodes) who were clinically diagnosed independently show common unique SERS spectral features in the urines collected just one day after transplant. SERS-based fiber-optic probe has excellent potential to be a bedside tool for early diagnosis of kidney transplant patients for timely medical intervention of patients at high risk of transplant dysfunction.

Design of near-infrared dyes for nonlinear optics: toward optical limiting applications at telecommunication wavelengths

NASA Astrophysics Data System (ADS)

Bellier, Quentin; Bouit, Pierre-Antoine; Kamada, Kenji; Feneyrou, Patrick; Malmström, E.; Maury, Olivier; Andraud, Chantal

2009-09-01

The rapid development of frequency-tunable pulsed lasers up to telecommunication wavelengths (1400-1600 nm) led to the design of new materials for nonlinear absorption in this spectral range. In this context, two families of near infra-red (NIR) chromophores, namely heptamethine cyanine and aza-borondipyrromethene (aza-bodipy) dyes were studied. In both cases, they show significant two-photon absorption (TPA) cross-sections in the 1400-1600 nm spectral range and display good optical power limiting (OPL) properties. OPL curves were interpreted on the basis of TPA followed by excited state absorption (ESA) phenomena. Finally these systems have several relevant properties like nonlinear absorption properties, gram scale synthesis and high solubility. In addition, they could be functionalized on several sites which open the way to numerous practical applications in biology, solid-state optical limiting and signal processing.

Directional radiation of Babinet-inverted optical nanoantenna integrated with plasmonic waveguide

NASA Astrophysics Data System (ADS)

Kim, Jineun; Roh, Young-Geun; Cheon, Sangmo; Jeong Kim, Un; Hwang, Sung Woo; Park, Yeonsang; Lee, Chang-Won

2015-07-01

We present a Babinet-inverted optical nanoantenna integrated with a plasmonic waveguide. Using an integrated nanoantenna, we can couple the plasmon guide mode in a metal-insulator-metal (MIM) structure into the resonant antenna feed directly. The resonantly excited feed slot then radiates to free space and generates a magnetic dipole-like far-field pattern. The coupling efficiency of the integrated nanoantenna is calculated as being approximately 19% using a three-dimensional finite-difference time-domain (3D FDTD) simulation. By adding an auxiliary groove structure along with the feed, the radiation direction can be controlled similar to an optical Yagi-Uda antenna. We also determine, both theoretically and experimentally, that groove depth plays a significant role to function groove structure as a reflector or a director. The demonstrated Babinet-inverted optical nanoantenna integrated with a plasmonic waveguide can be used as a “plasmonic via” in plasmonic nanocircuits.

Directional radiation of Babinet-inverted optical nanoantenna integrated with plasmonic waveguide.

PubMed

Kim, Jineun; Roh, Young-Geun; Cheon, Sangmo; Kim, Un Jeong; Hwang, Sung Woo; Park, Yeonsang; Lee, Chang-Won

2015-07-02

We present a Babinet-inverted optical nanoantenna integrated with a plasmonic waveguide. Using an integrated nanoantenna, we can couple the plasmon guide mode in a metal-insulator-metal (MIM) structure into the resonant antenna feed directly. The resonantly excited feed slot then radiates to free space and generates a magnetic dipole-like far-field pattern. The coupling efficiency of the integrated nanoantenna is calculated as being approximately 19% using a three-dimensional finite-difference time-domain (3D FDTD) simulation. By adding an auxiliary groove structure along with the feed, the radiation direction can be controlled similar to an optical Yagi-Uda antenna. We also determine, both theoretically and experimentally, that groove depth plays a significant role to function groove structure as a reflector or a director. The demonstrated Babinet-inverted optical nanoantenna integrated with a plasmonic waveguide can be used as a "plasmonic via" in plasmonic nanocircuits.

Directional radiation of Babinet-inverted optical nanoantenna integrated with plasmonic waveguide

PubMed Central

Kim, Jineun; Roh, Young-Geun; Cheon, Sangmo; Jeong Kim, Un; Hwang, Sung Woo; Park, Yeonsang; Lee, Chang-Won

2015-01-01

We present a Babinet-inverted optical nanoantenna integrated with a plasmonic waveguide. Using an integrated nanoantenna, we can couple the plasmon guide mode in a metal-insulator-metal (MIM) structure into the resonant antenna feed directly. The resonantly excited feed slot then radiates to free space and generates a magnetic dipole-like far-field pattern. The coupling efficiency of the integrated nanoantenna is calculated as being approximately 19% using a three-dimensional finite-difference time-domain (3D FDTD) simulation. By adding an auxiliary groove structure along with the feed, the radiation direction can be controlled similar to an optical Yagi-Uda antenna. We also determine, both theoretically and experimentally, that groove depth plays a significant role to function groove structure as a reflector or a director. The demonstrated Babinet-inverted optical nanoantenna integrated with a plasmonic waveguide can be used as a “plasmonic via” in plasmonic nanocircuits. PMID:26135115

Constraining the optical potential in the search for η-mesic 4He

NASA Astrophysics Data System (ADS)

Skurzok, M.; Moskal, P.; Kelkar, N. G.; Hirenzaki, S.; Nagahiro, H.; Ikeno, N.

2018-07-01

A consistent description of the dd →4Heη and dd → (4Heη)bound→ X cross sections was recently proposed with a broad range of real (V0) and imaginary (W0), η-4He optical potential parameters leading to a good agreement with the dd →4Heη data. Here we compare the predictions of the model below the η production threshold, with the WASA-at-COSY excitation functions for the dd →3HeNπ reactions to put stronger constraints on (V0 ,W0). The allowed parameter space (with |V0 | < ∼ 60 MeV and |W0 | < ∼ 7 MeV estimated at 90% CL) excludes most optical model predictions of η-4He nuclei except for some loosely bound narrow states.

Optical temperature sensing properties of Sm3+ doped SrWO4 phosphor

NASA Astrophysics Data System (ADS)

Song, Huiling; Han, Qun; Wang, Chao; Tang, Xiaoyun; Yan, Wenchuan; Chen, Yaofei; Zhao, Xueru; Jiang, Junfeng; Liu, Tiegen

2018-04-01

Sm3+ doped SrWO4 was synthesized by the high temperature solid-state reaction method to explore its possible application in optical thermometry. Under a 404 nm excitation, the fluorescence intensity ratios (FIRs) between the down conversion emissions of the Sm3+:4G5/2 → 6H5/2 (564 nm) to the Sm3+:4G5/2 → 6H7/2 (600 nm) and Sm3+:4G5/2 → 6H9/2 (647 nm), respectively, were measured as a function of temperature in the range of 300-573 K. A maximum temperature sensitivity of 0.016 K-1 at 300 K is achieved. The results indicate that the SrWO4:Sm3+ is a promising candidate for optical thermometry.

Optical rectification using geometrical field enhancement in gold nano-arrays

NASA Astrophysics Data System (ADS)

Piltan, S.; Sievenpiper, D.

2017-11-01

Conversion of photons to electrical energy has a wide variety of applications including imaging, solar energy harvesting, and IR detection. A rectenna device consists of an antenna in addition to a rectifying element to absorb the incident radiation within a certain frequency range. We designed, fabricated, and measured an optical rectifier taking advantage of asymmetrical field enhancement for forward and reverse currents due to geometrical constraints. The gold nano-structures as well as the geometrical parameters offer enhanced light-matter interaction at 382 THz. Using the Taylor expansion of the time-dependent current as a function of the external bias and oscillating optical excitation, we obtained responsivities close to quantum limit of operation. This geometrical approach can offer an efficient, broadband, and scalable solution for energy conversion and detection in the future.

Density gradient free electron collisionally excited X-ray laser

DOEpatents

Campbell, Edward M.; Rosen, Mordecai D.

1989-01-01

An operational X-ray laser (30) is provided that amplifies 3p-3s transition X-ray radiation along an approximately linear path. The X-ray laser (30) is driven by a high power optical laser. The driving line focused optical laser beam (32) illuminates a free-standing thin foil (34) that may be associated with a substrate (36) for improved structural integrity. This illumination produces a generally cylindrically shaped plasma having an essentially uniform electron density and temperature, that exists over a long period of time, and provides the X-ray laser gain medium. The X-ray laser (30) may be driven by more than one optical laser beam (32, 44). The X-ray laser (30) has been successfully demonstrated to function in a series of experimental tests.

Environmental effects on underwater optical transmission

NASA Astrophysics Data System (ADS)

Chu, Peter C.; Breshears, Brian F.; Cullen, Alexander J.; Hammerer, Ross F.; Martinez, Ramon P.; Phung, Thai Q.; Margolina, Tetyana; Fan, Chenwu

2017-05-01

Optical communication/detection systems have potential to get around some limitations of current acoustic communications and detection systems especially increased fleet and port security in noisy littoral waters. Identification of environmental effects on underwater optical transmission is the key to the success of using optics for underwater communication and detection. This paper is to answer the question "What are the transfer and correlation functions that relate measurements of hydrographic to optical parameters?" Hydrographic and optical data have been collected from the Naval Oceanographic Office survey ships with the High Intake Defined Excitation (HIDEX) photometer and sea gliders with optical back scattering sensor in various Navy interested areas such as the Arabian Gulf, Gulf of Oman, east Asian marginal seas, and Adriatic Sea. The data include temperature, salinity, bioluminescence, chlorophyll-a fluorescence, transmissivity at two different wavelengths (TRed at 670 nm, TBlue at 490 nm), and back scattering coefficient (bRed at 700 nm, bBlue at 470 nm). Transfer and correlation functions between the hydrographic and optical parameters are obtained. Bioluminescence and fluorescence maxima, transmissivity minimum with their corresponding depths, red and blue laser beam peak attenuation coefficients are identified from the optical profiles. Evident correlations are found between the ocean mixed layer depth and the blue and red laser beam peak attenuation coefficients, bioluminescence and fluorescence maxima in the Adriatic Sea, Arabian Gulf, Gulf of Oman, and Philippine Sea. Based on the observational data, an effective algorithm is recommended for solving the radiative transfer equation (RTE) for predicting underwater laser radiance.

Fluorescence Spectroscopic Properties of Normal and Abnormal Biomedical Materials

NASA Astrophysics Data System (ADS)

Pradhan, Asima

Steady state and time-resolved optical spectroscopy and native fluorescence is used to study the physical and optical properties occurring in diseased and non-diseased biological human tissue, in particular, cancer of the human breast, artery and the dynamics of a photosensitizer useful in photodynamic therapy. The main focus of the research is on the optical properties of cancer and atherosclerotic tissues as compared to their normal counterparts using the different luminescence based spectroscopic techniques such as steady state fluorescence, time-resolved fluorescence, excitation spectroscopy and phosphorescence. The excitation and steady-state spectroscopic fluorescence using visible excitation wavelength displays a difference between normal and malignant tissues. This difference is attributed to absorption of the emission by hemoglobin in normal tissues. This method using 488nm fails to distinguish neoplastic tissue such as benign tissues and tumors from malignant tumors. The time-resolved fluorescence at visible, near -uv and uv excitation wavelengths display non-exponential profiles which are significantly different for malignant tumors as compared to non-malignant tissues only with uv excitation. The differences observed with visible and near-uv excitation wavelengths are not as significant. The non-exponential profiles are interpreted as due to a combination of fluorophores along with the action of non-radiative processes. Low temperature luminescence studies confirm the occurrence of non-radiative decay processes while temporal studies of various relevant biomolecules indicate the probable fluorophores responsible for the observed signal in tissues. Phosphorescence from human tissues have been observed for the first time and lifetimes of a few hundred nanoseconds are measured for malignant and benign tissues. Time-resolved fluorescence studies of normal artery and atherosclerotic plaque have shown that a combination of two excitation wavelengths can distinguish fibrous and calcified atherosclerotic plaque from normal artery. A minor effort of the study involves the high intensity effects on the optical properties of the dye, doxycycline (a particular photosensitizer of the tetracycline group) occurring during relaxation when excited at different laser intensities. This study has been performed by observing the fluorescence lifetimes and quantum yields of DOTC at different excitation intensities. The results obtained support the sequential excited state absorption model.

Fast Electron Spectroscopy of Enhanced Plasmonic N anoantenna Resonances

NASA Astrophysics Data System (ADS)

Day, Jared K.

Surface plasmons are elementary excitations of the collective and coherent oscillations of conductive band electrons coupled with photons at the surface of metals. Surface plasmons of metallic nanostructures can efficiently couple to light making them a new class of optical antennas that can confine and control light at nanometer scale dimensions. Nanoscale optical antennas can be used to enhance the energy transfer between nanoscale systems and freely-propagating radiation. Plasmonic nanoantennas have already been used to enhance single molecule detection, diagnosis and treat cancer, harvest solar energy, to create metamaterials with new optical properties and to enhance photo-chemical reactions. The applications for plasmonic nanoantennas are only limited by the fundamental understanding of their unique optical properties and the rational design of new coupled antenna systems. It is therefore necessary to interrogate and image the local electromagnetic response of nanoantenna systems to establish intuition between near-field coupling dynamics and far-field optical properties. This thesis focuses on the characterization and enhancement of the longitudinal multipolar plasmonic resonances of Au nanorod nanoantennas. To better understand these resonances fast electron spectroscopy is used to both visualize and probe the near- and far-field properties of multipolar resonances of individual nanorods and more complex nanorod systems through cathodoluminescence (CL). CL intensity maps show that coupled nanorod systems enhance and alter nanorod resonances away from ideal resonant behavior creating hybridized longitudinal modes that expand and relax at controllable locations along the nanorod. These measurements show that complex geometries can strengthen and alter the local density of optical states for nanoantenna designs with more functionality and better control of localized electromagnetic fields. Finally, the electron excitations are compared to plane wave optical stimulation both experimentally and through Finite Difference Time Domain simulations to begin to develop a qualitative picture of how the local density of optical states affects the far-field optical scattering properties of plasmonic nanoantennas.

Multispectral photoacoustic method for the early detection and diagnosis of osteoporosis

NASA Astrophysics Data System (ADS)

Steinberg, Idan; Eyal, Avishay; Gannot, Israel

2013-03-01

Osteoporosis is a major health problem worldwide, with healthcare costs of billions of dollars annually. The risk of fracture depends on the bone mineral density (measured in clinical practice) as well as on the bone microstructure and functional status. Since pure ultrasonic methods can measure bone strength and spectroscopic optical methods can provide valuable functional information, a hybrid multispectral photoacoustic technique can be of great value. We have developed such a system based on a tunable Ti:Sapph laser at 750 - 950 nm, followed by an acousto-optic modulator to generate photoacoustic signals with frequencies of 0.5 - 2.5 MHz. Another system was based on two directly modulated 830nm laser diodes. The systems were used to photoacoustically excite the proximal end of a rat tibia. Spectrum analyzer with tracking generator was used for measuring both the amplitude and the phase at the distal end. Scanning along both the optical wavelength as well as the acoustic frequency enables full mapping of the bone transfer function. Analyzing this function along the wavelength axis allows deducing the gross biochemical composition related to the bone functional and pathological state. Analyzing the amplitude and phase along the acoustic frequency axis yields the speed of sound dispersion and the broadband ultrasonic attenuation - both have shown clinical relevance.

PREFACE: Ultrafast biophotonics Ultrafast biophotonics

NASA Astrophysics Data System (ADS)

Gu, Min; Reid, Derryck; Ben-Yakar, Adela

2010-08-01

The use of light to explore biology can be traced to the first observations of tissue made with early microscopes in the mid-seventeenth century, and has today evolved into the discipline which we now know as biophotonics. This field encompasses a diverse range of activities, each of which shares the common theme of exploiting the interaction of light with biological material. With the rapid advancement of ultrafast optical technologies over the last few decades, ultrafast lasers have increasingly found applications in biophotonics, to the extent that the distinctive new field of ultrafast biophotonics has now emerged, where robust turnkey ultrafast laser systems are facilitating cutting-edge studies in the life sciences to take place in everyday laboratories. The broad spectral bandwidths, precision timing resolution, low coherence and high peak powers of ultrafast optical pulses provide unique opportunities for imaging and manipulating biological systems. Time-resolved studies of bio-molecular dynamics exploit the short pulse durations from such lasers, while other applications such as optical coherence tomography benefit from the broad optical bandwidths possible by using super-continuum generation and additionally allowing for high speed imaging with speeds as high as 47 000 scans per second. Continuing progress in laser-system technology is accelerating the adoption of ultrafast techniques across the life sciences, both in research laboratories and in clinical applications, such as laser-assisted in situ keratomileusis (LASIK) eye surgery. Revolutionizing the field of optical microscopy, two-photon excitation fluorescence (TPEF) microscopy has enabled higher spatial resolution with improved depth penetration into biological specimens. Advantages of this nonlinear optical process include: reduced photo-interactions, allowing for extensive imaging time periods; simultaneously exciting multiple fluorescent molecules with only one excitation wavelength; and reduced chromatic aberration effects. These extensive advantages have led to further exploration of nonlinear processes including second-harmonic generation (SHG) microscopy and third-harmonic generation (THG) microscopy. Second-harmonic generation has provided biologists with an extremely powerful tool for generating contrast in biological imaging, with the additional benefit of non-invasive three-dimensional imaging. The recent popularity of THG microscopy is largely due to the fact that three-dimensional imaging is achievable without the need for any labels, but rather relying on the intrinsic properties of the biological specimen itself. This optical nonlinear technique has attracted much attention recently from the biological community due to its non-invasive capabilities. Users of ultrafast lasers in the biological and medical fields are becoming a fast-growing community, employing pulse-shaping microscopy, resolution-enhancing microscopy techniques, linear and nonlinear micro-spectroscopy, functional deep-tissue imaging, optical coherence tomography, nonlinear fluorescence microscopy, molecular imaging and control, harmonic microscopy and femtosecond lifetime imaging, for cutting-edge research concerning the interaction of light with biological dynamics. The adaptability of ultrafast lasers to interact with a large array of materials through nonlinear excitation has enabled precise control of laser fluence allowing for highly localized material interactions, permitting micro-structured fabricated surfaces. The resultant multi-dimensional fabricated micro-structures are capable of replicating and/or manipulating microenvironments for controlled cell biology. In this special issue of Journal of Optics readers have a chance to view a collection of new contributions to the growing research field of ultrafast biophotonics. They are presented with recent advances in ultrafast technology applied to biological and medical investigations, where topics include advances in the visualization and identification of photo-reaction dynamics of biological functions under relevant physiological conditions, theoretically proposed imaging designs for obtaining super-resolved optical sectioned images in single exposures and fabricated micro-structured surfaces for biological micro-environments. We hope the collection will stimulate innovative new research in this growing field by showcasing new techniques for the visualization and manipulation of complex biological systems using linear and and nonlinear optical processes. Professor Min Gu would like to acknowledge Dr Betty Kouskousis for her contribution and support towards this editorial.

Palette of fluorinated voltage-sensitive hemicyanine dyes

PubMed Central

Yan, Ping; Acker, Corey D.; Zhou, Wen-Liang; Lee, Peter; Bollensdorff, Christian; Negrean, Adrian; Lotti, Jacopo; Sacconi, Leonardo; Antic, Srdjan D.; Kohl, Peter; Mansvelder, Huibert D.; Pavone, Francesco S.; Loew, Leslie M.

2012-01-01

Optical recording of membrane potential permits spatially resolved measurement of electrical activity in subcellular regions of single cells, which would be inaccessible to electrodes, and imaging of spatiotemporal patterns of action potential propagation in excitable tissues, such as the brain or heart. However, the available voltage-sensitive dyes (VSDs) are not always spectrally compatible with newly available optical technologies for sensing or manipulating the physiological state of a system. Here, we describe a series of 19 fluorinated VSDs based on the hemicyanine class of chromophores. Strategic placement of the fluorine atoms on the chromophores can result in either blue or red shifts in the absorbance and emission spectra. The range of one-photon excitation wavelengths afforded by these new VSDs spans 440–670 nm; the two-photon excitation range is 900–1,340 nm. The emission of each VSD is shifted by at least 100 nm to the red of its one-photon excitation spectrum. The set of VSDs, thus, affords an extended toolkit for optical recording to match a broad range of experimental requirements. We show the sensitivity to voltage and the photostability of the new VSDs in a series of experimental preparations ranging in scale from single dendritic spines to whole heart. Among the advances shown in these applications are simultaneous recording of voltage and calcium in single dendritic spines and optical electrophysiology recordings using two-photon excitation above 1,100 nm. PMID:23169660

Reconfigurable lateral optical force achieved by selectively exciting plasmonic dark modes near Fano resonance

NASA Astrophysics Data System (ADS)

Chen, Huajin; Ye, Qian; Zhang, Yiwen; Shi, Lei; Liu, Shiyang; Jian, Zi; Lin, Zhifang

2017-08-01

We demonstrate a reconfigurable lateral optical force (OF) on a plasmonic nanoparticle immersed in a simple optical field invariant along the lateral direction and formed by two interfering plane waves. This lateral OF is shown, from the multipolar expansion technique, attributed to several coupling channels established between multiple multipoles excited on a plasmonic nanoparticle, in particular, the adjacent electric multipole modes that bring about the Fano interferences, which can substantially enhance the lateral scattering asymmetry, leading to an augmented lateral OF comparable to the longitudinal OF. More importantly, by engineering Fano interference either intrinsically through particle size or extrinsically through selectively exciting narrow plasmonic dark modes the direction of the lateral OF is reversibly switchable. The lateral OF can even be modulated continuously from positive to negative by controlling the incident angle of the interfering plane waves due to the variation of relative phase of the excited plasmonic dark modes near Fano resonance, facilitating the plasmonic nanoparticle as a controllable conveyor as well as the optical selection and separation. Besides, a fundamental and counterintuitive physical consequence emerges in that the simple proportional relation between the lateral OF and the Belinfante spin momentum derived in the small particle limit breaks down when the Fano interference comes into play, in particular, a negative lateral OF opposite the Belinfante spin momentum can be induced by properly controlling the selective excitation.

Functional metasurfaces based on metallic and dielectric subwavelength slits and stripes array

NASA Astrophysics Data System (ADS)

Guo, Yinghui; Pu, Mingbo; Li, Xiong; Ma, Xiaoliang; Gao, Ping; Wang, Yanqin; Luo, Xiangang

2018-04-01

Starting with the early works of extraordinary optical transmission and extraordinary Young’s interference, researchers have been fascinated by the unusual optical properties displayed by metallic holes/slits and subsequently found similar abnormities in dielectric counterparts. Benefiting from the shrinking wavelength of surface plasmon polaritons excited in metallic slits and high refractive index of dielectric stripes, one can realize local phase modulation and approach desired dispersion by engineering the geometries of a slits and stripes array. In this review, we review recent developments in functional metasurfaces composed of various metallic and dielectric subwavelength slits and stripes arrays, with special emphasis on achromatic, ultra-broadband, quasi-continuous, multifunctional and reconfigurable metasurfaces. Particular attention is paid to provide insight into the design strategies for these devices. Finally, we give an outlook of the development in this fascinating area.

Molecular design and theoretical characterization of benzodithiophene based organic photovoltaic materials

NASA Astrophysics Data System (ADS)

Bhattacharya, Labanya; Sahu, Sridhar

2018-05-01

Two different oligomers, containing methyl substituted Benzodithiophene (BDT) as donor unit, fluorinated thiophene as the π-bridge unit and two different kinds of acceptors based on fluorinated benzothiadiazole, fluorinated benzoselenadiazole units are designed for bulk heterojunction (BHJ) organic solar cell (OSC). The ground and excited state properties of those donor-π-acceptor-π-donor (D-π-A-π-D) oligomeric configurations are characterized via density functional (DFT) and time dependent density functional theory (TD-DFT). The parameters such as dipole moment (ρ), chemical potential (µ), electronegativity (χ), frontier molecular orbital (FMO) analysis, HOMO-LUMO gap, open circuit voltage (Voc) and driving force (ΔE) are calculated to analyze geometrical, electronic structural, quantum chemical and photovoltaic properties of the compounds. In addition, optical absorption spectra are also presented for the optical characterization of the compounds.

The realization of the dipole (γ, γ) method and its application to determine the absolute optical oscillator strengths of helium.

PubMed

Xu, Long-Quan; Liu, Ya-Wei; Kang, Xu; Ni, Dong-Dong; Yang, Ke; Hiraoka, Nozomu; Tsuei, Ku-Ding; Zhu, Lin-Fan

2015-12-17

The dipole (γ, γ) method, which is the inelastic x-ray scattering operated at a negligibly small momentum transfer, is proposed and realized to determine the absolute optical oscillator strengths of the vanlence-shell excitations of atoms and molecules. Compared with the conventionally used photoabsorption method, this new method is free from the line saturation effect, which can seriously limit the accuracies of the measured photoabsorption cross sections for discrete transitions with narrow natural linewidths. Furthermore, the Bethe-Born conversion factor of the dipole (γ, γ) method varies much more slowly with the excitation energy than does that of the dipole (e, e) method. Absolute optical oscillator strengths for the excitations of 1s(2) → 1 snp(n = 3-7) of atomic helium have been determined using the high-resolution dipole (γ, γ) method, and the excellent agreement of the present measurements with both those measured by the dipole (e, e) method and the previous theoretical calculations indicates that the dipole (γ, γ) method is a powerful tool to measure the absolute optical oscillator strengths of the valence-shell excitations of atoms and molecules.

Electron-related linear and nonlinear optical responses in vertically coupled triangular quantum dots

NASA Astrophysics Data System (ADS)

Martínez-Orozco, J. C.; Mora-Ramos, M. E.; Duque, C. A.

2014-11-01

The conduction band states of GaAs-based vertically coupled double triangular quantum dots in two dimensions are investigated within the effective mass and parabolic approximation, using a diagonalization procedure to solve the corresponding Schrödinger-like equation. The effect of an externally applied static electric field is included in the calculation, and the variation of the lowest confined energy levels as a result of the change of the field strength is reported for different geometrical setups. The linear and nonlinear optical absorptions and the relative change of the refractive index, associated with the energy transition between the ground and the first excited state in the system, are studied as a function of the incident light frequency for distinct configurations of inter-dot distance and electric field intensities. The blueshift of the resonant absorption peaks is detected as a consequence of the increment in the field intensity, whereas the opposite effect is obtained from the increase of inter-dot vertical distance. It is also shown that for large enough values of the electric field there is a quenching of the optical absorption due to field-induced change of symmetry of the first excited state wavefunction, in the case of triangular dots of equal shape and size.

Dynamic Response of an Optomechanical System to a Stationary Random Excitation in the Time Domain

DOE PAGES

Palmer, Jeremy A.; Paez, Thomas L.

2011-01-01

Modern electro-optical instruments are typically designed with assemblies of optomechanical members that support optics such that alignment is maintained in service environments that include random vibration loads. This paper presents a nonlinear numerical analysis that calculates statistics for the peak lateral response of optics in an optomechanical sub-assembly subject to random excitation of the housing. The work is unique in that the prior art does not address peak response probability distribution for stationary random vibration in the time domain for a common lens-retainer-housing system with Coulomb damping. Analytical results are validated by using displacement response data from random vibration testingmore » of representative prototype sub-assemblies. A comparison of predictions to experimental results yields reasonable agreement. The Type I Asymptotic form provides the cumulative distribution function for peak response probabilities. Probabilities are calculated for actual lens centration tolerances. The probability that peak response will not exceed the centration tolerance is greater than 80% for prototype configurations where the tolerance is high (on the order of 30 micrometers). Conversely, the probability is low for those where the tolerance is less than 20 micrometers. The analysis suggests a design paradigm based on the influence of lateral stiffness on the magnitude of the response.« less

Separating Bulk and Surface Contributions to Electronic Excited-State Processes in Hybrid Mixed Perovskite Thin Films via Multimodal All-Optical Imaging.

PubMed

Simpson, Mary Jane; Doughty, Benjamin; Das, Sanjib; Xiao, Kai; Ma, Ying-Zhong

2017-07-20

A comprehensive understanding of electronic excited-state phenomena underlying the impressive performance of solution-processed hybrid halide perovskite solar cells requires access to both spatially resolved electronic processes and corresponding sample morphological characteristics. Here, we demonstrate an all-optical multimodal imaging approach that enables us to obtain both electronic excited-state and morphological information on a single optical microscope platform with simultaneous high temporal and spatial resolution. Specifically, images were acquired for the same region of interest in thin films of chloride containing mixed lead halide perovskites (CH 3 NH 3 PbI 3-x Cl x ) using femtosecond transient absorption, time-integrated photoluminescence, confocal reflectance, and transmission microscopies. Comprehensive image analysis revealed the presence of surface- and bulk-dominated contributions to the various images, which describe either spatially dependent electronic excited-state properties or morphological variations across the probed region of the thin films. These results show that PL probes effectively the species near or at the film surface.

Two-Photon Optical Properties of Near-Infrared Dyes at 1.55 microns Excitation

PubMed Central

Berezin, Mikhail; Zhan, Chun; Lee, Hyeran; Joo, Chulmin; Akers, Walter; Yazdanfar, Siavash; Achilefu, Samuel

2011-01-01

Two-photon (2P) optical properties of cyanine dyes were evaluated using a 2P fluorescence spectrophotometer with 1.55 μm excitation. We report the 2P characteristics of common NIR polymethine dyes, including their 2P action cross-sections and the 2P excited fluorescence lifetime. One of the dyes, DTTC showed the highest 2P action cross-section (~103 ± 19 GM) and relatively high 2P excited fluorescence lifetime and can be used as a scaffold for the synthesis of 2P molecular imaging probes. The 2P action cross-section of DTTC and the lifetime were also highly sensitive to the solvent polarity, providing other additional parameters for its use in optical imaging and the mechanism for probing environmental factors Overall, this study demonstrated the quantitative measurement of 2P properties of NIR dyes and established the foundation for designing molecular probes for 2P imaging applications in the NIR region. PMID:21866928

Resonances in the optical response of a slab with time-periodic dielectric function {epsilon}(t)

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

Zurita-Sanchez, Jorge R.; Halevi, P.

2010-05-15

We demonstrate that the optical response of a periodically modulated dynamic slab exhibits infinite resonances for frequencies {omega}=({Omega}/2)(2l+1), namely, odd multiples of one-half of the modulating frequency {Omega} of the dielectric function {epsilon}(t). These frequencies coincide partially with the usual condition of parametric amplification. However, the resonances occur only for certain normalized slab thicknesses L{sub R}. These resonances follow from detailed numerical studies based on our recent paper [Zurita-Sanchez, Halevi, and Cervantes-Gonzalez, Phys. Rev. A 79, 053821 (2009)]. As the thickness L nearly matches a resonance thickness L{sub R}, the amplitudes of counterpropagating modes in the slab obey a conditionmore » implying that both have the same modulus and their phases match a condition related to L{sub R} and the bulk wave vectors. When this condition is met, the electric field profile inside the slab is a superposition of standing waves with odd and even symmetries, and the reflection and transmission coefficients can reach great values and become infinite at exact resonance. Numerical simulations of the optical response are shown for a sinusoidal {epsilon}(t) with either moderate or strong modulation. As expected, as the modulation strength increases, higher-order harmonics {omega}-n{Omega} (n=0,{+-}1,{+-}2,...) become more noticeable, and short-wavelength bulk modes contribute significantly. However, we found that, regardless of the excitation frequency {omega}=({Omega}/2)(2l+1), the dominant spectral component of the generated fields is {Omega}/2. Also, as the excitation frequency increases, the parity of the standing waves is conserved.« less

Physical limits to autofluorescence signals in vivo recordings in the rat olfactory bulb: a Monte Carlo study

NASA Astrophysics Data System (ADS)

L'Heureux, B.; Gurden, H.; Pinot, L.; Mastrippolito, R.; Lefebvre, F.; Lanièce, P.; Pain, F.

2007-07-01

Understanding the cellular mechanisms of energy supply to neurons following physiological activation is still challenging and has strong implications to the interpretation of clinical functional images based on metabolic signals such as Blood Oxygen Level Dependent Magnetic Resonance Imaging or 18F-Fluorodexoy-Glucose Positron Emission Tomography. Intrinsic Optical Signal Imaging provides with high spatio temporal resolution in vivo imaging in the anaesthetized rat. In that context, intrinsic signals are mainly related to changes in the optical absorption of haemoglobin depending on its oxygenation state. This technique has been validated for imaging of the rat olfactory bulb, providing with maps of the actived olfactory glomeruli, the functional modules involved in the first step of olfactory coding. A complementary approach would be autofluorescence imaging relying on the fluorescence properties of endogenous Flavin Adenine Dinucleotide (FAD) or Nicotinamide Adenine Dinucleotide (NADH) both involved in intracellular metabolic pathways. The purpose of the present study was to investigate the feasibility of in vivo autofluorescence imaging in the rat olfactory bulb. We performed standard Monte Carlo simulations of photons scattering and absorption at the excitation and emission wavelengths of FAD and NADH fluorescence. Characterization of the fluorescence distribution in the glomerulus, effect of hemoglobin absorption at the excitation and absorption wavelengths as well as the effect of the blurring due to photon scattering and the depth of focus of the optical apparatus have been studied. Finally, optimal experimental parameters are proposed to achieve in vivo validation of the technique in the rat olfactory bulb.

Organic Micro/Nanoscale Lasers.

PubMed

Zhang, Wei; Yao, Jiannian; Zhao, Yong Sheng

2016-09-20

Micro/nanoscale lasers that can deliver intense coherent light signals at (sub)wavelength scale have recently captured broad research interest because of their potential applications ranging from on-chip information processing to high-throughput sensing. Organic molecular materials are a promising kind of ideal platform to construct high-performance microlasers, mainly because of their superiority in abundant excited-state processes with large active cross sections for high gain emissions and flexibly assembled structures for high-quality microcavities. In recent years, ever-increasing efforts have been dedicated to developing such organic microlasers toward low threshold, multicolor output, broadband tunability, and easy integration. Therefore, it is increasingly important to summarize this research field and give deep insight into the structure-property relationships of organic microlasers to accelerate the future development. In this Account, we will review the recent advances in organic miniaturized lasers, with an emphasis on tunable laser performances based on the tailorable microcavity structures and controlled excited-state gain processes of organic materials toward integrated photonic applications. Organic π-conjugated molecules with weak intermolecular interactions readily assemble into regular nanostructures that can serve as high-quality optical microcavities for the strong confinement of photons. On the basis of rational material design, a series of optical microcavities with different structures have been controllably synthesized. These microcavity nanostructures can be endowed with effective four-level dynamic gain processes, such as excited-state intramolecular charge transfer, excited-state intramolecular proton transfer, and excimer processes, that exhibit large dipole optical transitions for strongly active gain behaviors. By tailoring these excited-state processes with molecular/crystal engineering and external stimuli, people have effectively modulated the performances of organic micro/nanolasers. Furthermore, by means of controlled assembly and tunable laser performances, efficient outcoupling of microlasers has been successfully achieved in various organic hybrid microstructures, showing considerable potential for the integrated photonic applications. This Account starts by presenting an overview of the research evolution of organic microlasers in terms of microcavity resonators and energy-level gain. Then a series of strategies to tailor the microcavity structures and excited-state dynamics of organic nanomaterials for the modulation of lasing performances are highlighted. In the following part, we introduce the construction and advanced photonic functionalities of organic-microlaser-based hybrid structures and their applications in integrated nanophotonics. Finally, we provide our outlook on the current challenges as well as the future development of organic microlasers. It is anticipated that this Account will provide inspiration for the development of miniaturized lasers with desired performances by tailoring of excited-state processes and microcavity structures toward integrated photonic applications.

Ab Initio Study of Electronic Excitation Effects on SrTiO 3

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

Zhao, Shijun; Zhang, Yanwen; Weber, William J.

Interaction of energetic ions or lasers with solids often induces electronic excitations that may modify material properties significantly. In this study, effects of electronic excitations on strontium titanate SrTiO 3 (STO) are investigated based on first-principles calculations. The lattice structure, electronic properties, lattice vibrational frequencies, and dynamical stabilities are studied in detail. The results suggest that electronic excitation induces charge redistribution that is mainly observed in Ti–O bonds. The electronic band gap increases with increasing electronic excitation, as excitation mainly induces depopulation of Ti 3d states. Phonon analysis indicates that there is a large phonon band gap induced by electronicmore » excitation because of the changes in the vibrational properties of Ti and O atoms. In addition, a new peak appears in the phonon density of states with imaginary frequencies, an indication of lattice instability. Further dynamics simulations confirm that STO undergoes transition to an amorphous structure under strong electronic excitations. In conclusion, the optical properties of STO under electronic excitation are consistent with the evolution of atomic and electronic structures, which suggests a possibility to probe the properties of STO in nonequilibrium state using optical measurement.« less

Ab Initio Study of Electronic Excitation Effects on SrTiO 3

DOE PAGES

Zhao, Shijun; Zhang, Yanwen; Weber, William J.

2017-11-14

Interaction of energetic ions or lasers with solids often induces electronic excitations that may modify material properties significantly. In this study, effects of electronic excitations on strontium titanate SrTiO 3 (STO) are investigated based on first-principles calculations. The lattice structure, electronic properties, lattice vibrational frequencies, and dynamical stabilities are studied in detail. The results suggest that electronic excitation induces charge redistribution that is mainly observed in Ti–O bonds. The electronic band gap increases with increasing electronic excitation, as excitation mainly induces depopulation of Ti 3d states. Phonon analysis indicates that there is a large phonon band gap induced by electronicmore » excitation because of the changes in the vibrational properties of Ti and O atoms. In addition, a new peak appears in the phonon density of states with imaginary frequencies, an indication of lattice instability. Further dynamics simulations confirm that STO undergoes transition to an amorphous structure under strong electronic excitations. In conclusion, the optical properties of STO under electronic excitation are consistent with the evolution of atomic and electronic structures, which suggests a possibility to probe the properties of STO in nonequilibrium state using optical measurement.« less

Excitation of Cy5 in self-assembled lipid bilayers using optical microresonators

NASA Astrophysics Data System (ADS)

Freeman, Lindsay M.; Li, Su; Dayani, Yasaman; Choi, Hong-Seok; Malmstadt, Noah; Armani, Andrea M.

2011-04-01

Due to their sensitivity and temporal response, optical microresonators are used extensively in the biosensor arena, particularly in the development of label-free diagnostics and measurement of protein kinetics. In the present letter, we investigate using microcavities to probe molecules within biomimetic membranes. Specifically, a method for self-assembling lipid bilayers on spherical microresonators is developed and the bilayer-nature is verified. Subsequently, the microcavity is used to excite a Cy5-conjugated lipid located within the bilayer while the optical performance of the microcavity is characterized. The emission wavelength of the dye and the optical behavior of the microcavity agree with theoretical predictions.

Creating optical near-field orbital angular momentum in a gold metasurface.

PubMed

Chen, Ching-Fu; Ku, Chen-Ta; Tai, Yi-Hsin; Wei, Pei-Kuen; Lin, Heh-Nan; Huang, Chen-Bin

2015-04-08

Nanocavities inscribed in a gold thin film are optimized and designed to form a metasurface. We demonstrate both numerically and experimentally the creation of surface plasmon (SP) vortex carrying orbital angular momentum in the metasurface under linearly polarized optical excitation that carries no optical angular momentum. Moreover, depending on the orientation of the exciting linearly polarized light, we show that the metasurface is capable of providing dynamic switching between SP vortex formation or SP subwavelength focusing. The resulting SP intensities are experimentally measured using a near-field scanning optical microscope and are found in excellent quantitative agreements as compared to the numerical results.

Phonon-assisted nonlinear optical processes in ultrashort-pulse pumped optical parametric amplifiers

NASA Astrophysics Data System (ADS)

Isaienko, Oleksandr; Robel, István

2016-03-01

Optically active phonon modes in ferroelectrics such as potassium titanyl phosphate (KTP) and potassium titanyl arsenate (KTA) in the ~7-20 THz range play an important role in applications of these materials in Raman lasing and terahertz wave generation. Previous studies with picosecond pulse excitation demonstrated that the interaction of pump pulses with phonons can lead to efficient stimulated Raman scattering (SRS) accompanying optical parametric oscillation or amplification processes (OPO/OPA), and to efficient polariton-phonon scattering. In this work, we investigate the behavior of infrared OPAs employing KTP or KTA crystals when pumped with ~800-nm ultrashort pulses of duration comparable to the oscillation period of the optical phonons. We demonstrate that under conditions of coherent impulsive Raman excitation of the phonons, when the effective χ(2) nonlinearity cannot be considered instantaneous, the parametrically amplified waves (most notably, signal) undergo significant spectral modulations leading to an overall redshift of the OPA output. The pump intensity dependence of the redshifted OPA output, the temporal evolution of the parametric gain, as well as the pump spectral modulations suggest the presence of coupling between the nonlinear optical polarizations PNL of the impulsively excited phonons and those of parametrically amplified waves.

Photo-induced-heat localization on nanostructured metallic glasses

NASA Astrophysics Data System (ADS)

Uzun, Ceren; Kahler, Niloofar; Grave de Peralta, Luis; Kumar, Golden; Bernussi, Ayrton A.

2017-09-01

Materials with large photo-thermal energy conversion efficiency are essential for renewable energy applications. Photo-excitation is an effective approach to generate controlled and localized heat at relatively low excitation optical powers. However, lateral heat diffusion to the surrounding illuminated areas accompanied by low photo-thermal energy conversion efficiency remains a challenge for metallic surfaces. Surface nanoengineering has proven to be a successful approach to further absorption and heat generation. Here, we show that pronounced spatial heat localization and high temperatures can be achieved with arrays of amorphous metallic glass nanorods under infrared optical illumination. Thermography measurements revealed marked temperature contrast between illuminated and non-illuminated areas even under low optical power excitation conditions. This attribute allowed for generating legible photo-induced thermal patterns on textured metallic glass surfaces.

A Reversible DNA Logic Gate Platform Operated by One- and Two-Photon Excitations.

PubMed

Tam, Dick Yan; Dai, Ziwen; Chan, Miu Shan; Liu, Ling Sum; Cheung, Man Ching; Bolze, Frederic; Tin, Chung; Lo, Pik Kwan

2016-01-04

We demonstrate the use of two different wavelength ranges of excitation light as inputs to remotely trigger the responses of the self-assembled DNA devices (D-OR). As an important feature of this device, the dependence of the readout fluorescent signals on the two external inputs, UV excitation for 1 min and/or near infrared irradiation (NIR) at 800 nm fs laser pulses, can mimic function of signal communication in OR logic gates. Their operations could be reset easily to its initial state. Furthermore, these DNA devices exhibit efficient cellular uptake, low cytotoxicity, and high bio-stability in different cell lines. They are considered as the first example of a photo-responsive DNA logic gate system, as well as a biocompatible, multi-wavelength excited system in response to UV and NIR. This is an important step to explore the concept of photo-responsive DNA-based systems as versatile tools in DNA computing, display devices, optical communication, and biology. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Excitation of epsilon-near-zero resonance in ultra-thin indium tin oxide shell embedded nanostructured optical fiber.

PubMed

Minn, Khant; Anopchenko, Aleksei; Yang, Jingyi; Lee, Ho Wai Howard

2018-02-05

We report a novel optical waveguide design of a hollow step index fiber modified with a thin layer of indium tin oxide (ITO). We show an excitation of highly confined waveguide mode in the proposed fiber near the wavelength where permittivity of ITO approaches zero. Due to the high field confinement within thin ITO shell inside the fiber, the epsilon-near-zero (ENZ) mode can be characterized by a peak in modal loss of the hybrid waveguide. Our results show that such in-fiber excitation of ENZ mode is due to the coupling of the guided core mode to the thin-film ENZ mode. We also show that the phase matching wavelength, where the coupling takes place, varies depending on the refractive index of the constituents inside the central bore of the fiber. These ENZ nanostructured optical fibers have many potential applications, for example, in ENZ nonlinear and magneto-optics, as in-fiber wavelength-dependent filters, and as subwavelength fluid channel for optical and bio-photonic sensing.

LASER FLUORESCENCE EEM PROBE FOR CONE PENETROMETER POLLUTION ANALYSIS

EPA Science Inventory

A fiber optic LIF (Laser induced fluorescence) EEM (Excitation emission matrix) instrument for CPT deployment has been successfully developed and field tested. The system employs a Nd: YAG laser and Raman shifter as a rugged field portable excitation source. This excitation sou...

Electron photodetachment from gas phase peptide dianions. Relation with optical absorption properties.

PubMed

Joly, Laure; Antoine, Rodolphe; Broyer, Michel; Lemoine, Jérôme; Dugourd, Philippe

2008-02-07

Electron detachment from peptide dianions is studied as a function of the laser wavelength. The first step for the detachment is a resonant electronic excitation of the dianions. Electronic excitation spectra are reported for three peptides, including gramicidin. A comparative study of the detachment yield for 13 peptides was performed at 260 nm and at 220 nm. At 260 nm, the detachment yield is mainly driven by the sum of the absorption coefficients of the aromatic amino acids that are contained in the peptide. At 220 nm, no direct relation is observed between the electron photodetachement yields and the sum of absorption efficiencies. At this wavelength, the sequence and the structure of the peptide may have an influence on the photodetachment process.

Photoelectron Energy Loss in Al(002) Revisited: Retrieval of the Single Plasmon Loss Energy Distribution by a Fourier Transform Method

NASA Astrophysics Data System (ADS)

Santana, Victor Mancir da Silva; David, Denis; de Almeida, Jailton Souza; Godet, Christian

2018-06-01

A Fourier transform (FT) algorithm is proposed to retrieve the energy loss function (ELF) of solid surfaces from experimental X-ray photoelectron spectra. The intensity measured over a broad energy range towards lower kinetic energies results from convolution of four spectral distributions: photoemission line shape, multiple plasmon loss probability, X-ray source line structure and Gaussian broadening of the photoelectron analyzer. The FT of the measured XPS spectrum, including the zero-loss peak and all inelastic scattering mechanisms, being a mathematical function of the respective FT of X-ray source, photoemission line shape, multiple plasmon loss function, and Gaussian broadening of the photoelectron analyzer, the proposed algorithm gives straightforward access to the bulk ELF and effective dielectric function of the solid, assuming identical ELF for intrinsic and extrinsic plasmon excitations. This method is applied to aluminum single crystal Al(002) where the photoemission line shape has been computed accurately beyond the Doniach-Sunjic approximation using the Mahan-Wertheim-Citrin approach which takes into account the density of states near the Fermi level; the only adjustable parameters are the singularity index and the broadening energy D (inverse hole lifetime). After correction for surface plasmon excitations, the q-averaged bulk loss function, q , of Al(002) differs from the optical value Im[- 1 / ɛ( E, q = 0)] and is well described by the Lindhard-Mermin dispersion relation. A quality criterion of the inversion algorithm is given by the capability of observing weak interband transitions close to the zero-loss peak, namely at 0.65 and 1.65 eV in ɛ( E, q) as found in optical spectra and ab initio calculations of aluminum.

Photoelectron Energy Loss in Al(002) Revisited: Retrieval of the Single Plasmon Loss Energy Distribution by a Fourier Transform Method

NASA Astrophysics Data System (ADS)

Santana, Victor Mancir da Silva; David, Denis; de Almeida, Jailton Souza; Godet, Christian

2018-04-01

A Fourier transform (FT) algorithm is proposed to retrieve the energy loss function (ELF) of solid surfaces from experimental X-ray photoelectron spectra. The intensity measured over a broad energy range towards lower kinetic energies results from convolution of four spectral distributions: photoemission line shape, multiple plasmon loss probability, X-ray source line structure and Gaussian broadening of the photoelectron analyzer. The FT of the measured XPS spectrum, including the zero-loss peak and all inelastic scattering mechanisms, being a mathematical function of the respective FT of X-ray source, photoemission line shape, multiple plasmon loss function, and Gaussian broadening of the photoelectron analyzer, the proposed algorithm gives straightforward access to the bulk ELF and effective dielectric function of the solid, assuming identical ELF for intrinsic and extrinsic plasmon excitations. This method is applied to aluminum single crystal Al(002) where the photoemission line shape has been computed accurately beyond the Doniach-Sunjic approximation using the Mahan-Wertheim-Citrin approach which takes into account the density of states near the Fermi level; the only adjustable parameters are the singularity index and the broadening energy D (inverse hole lifetime). After correction for surface plasmon excitations, the q-averaged bulk loss function, q , of Al(002) differs from the optical value Im[- 1 / ɛ(E, q = 0)] and is well described by the Lindhard-Mermin dispersion relation. A quality criterion of the inversion algorithm is given by the capability of observing weak interband transitions close to the zero-loss peak, namely at 0.65 and 1.65 eV in ɛ(E, q) as found in optical spectra and ab initio calculations of aluminum.

Excitation of photonic atoms (dielectric microspheres) on optical fibers: application to room-temperature persistent spectral hole burning

NASA Astrophysics Data System (ADS)

Serpenguzel, Ali; Arnold, Stephen; Griffel, Giora

1995-05-01

Recently, photonic atoms (dielectric microspheres) have enjoyed the attention of the optical spectroscopy community. A variety of linear and nonlinear optical processes have been observed in liquid microdroplets. But solid state photonic devices using these properties are scarce. A first of these applications is the room temperature microparticle hole-burning memory. New applications can be envisioned if microparticle resonances can be coupled to traveling waves in optical fibers. In this paper we demonstrate the excitation of narrow morphology dependent resonances of microparticles placed on an optical fiber. Furthermore we reveal a model for this process which describes the coupling efficiency in terms of the geometrical and material properties of the microparticle-fiber system.

Efficient photoconductive terahertz detector with all-dielectric optical metasurface

NASA Astrophysics Data System (ADS)

Mitrofanov, Oleg; Siday, Thomas; Thompson, Robert J.; Luk, Ting Shan; Brener, Igal; Reno, John L.

2018-05-01

We designed an optically thin photoconductive channel as an all-dielectric metasurface comprising an array of low-temperature grown GaAs nanobeams and a sub-surface distributed Bragg reflector. The metasurface exhibited enhanced optical absorption, and it was integrated into a photoconductive THz detector, which showed high efficiency and sensitivity as a result. The detector produced photocurrents over one order of magnitude higher compared to a similar detector with an unstructured surface with only 0.5 mW of optical excitation while exhibiting high dark resistance required for low-noise detection in THz time-domain spectroscopy and imaging. At that level of optical excitation, the metasurface detector showed a high signal to noise ratio of 106. The detector showed saturation above that level.

Ultrafast optical pulse delivery with fibers for nonlinear microscopy

PubMed Central

Kim, Daekeun; Choi, Heejin; Yazdanfar, Siavash; So, Peter T. C.

2008-01-01

Nonlinear microscopies including multiphoton excitation fluorescence microscopy and multiple-harmonic generation microscopy have recently gained popularity for cellular and tissue imaging. The optimization of these imaging methods for minimally invasive use will require optical fibers to conduct light into tight space where free space delivery is difficult. The delivery of high peak power laser pulses with optical fibers is limited by dispersion resulting from nonlinear refractive index responses. In this paper, we characterize a variety of commonly used optical fibers in terms of how they affect pulse profile and imaging performance of nonlinear microscopy; the following parameters are quantified: spectral bandwidth and temporal pulse width, two-photon excitation efficiency, and optical resolution. A theoretical explanation for the measured performance of these is also provided. PMID:18816597

Electron-phonon relaxation and excited electron distribution in gallium nitride

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

Zhukov, V. P.; Donostia International Physics Center; Tyuterev, V. G., E-mail: valtyut00@mail.ru

2016-08-28

We develop a theory of energy relaxation in semiconductors and insulators highly excited by the long-acting external irradiation. We derive the equation for the non-equilibrium distribution function of excited electrons. The solution for this function breaks up into the sum of two contributions. The low-energy contribution is concentrated in a narrow range near the bottom of the conduction band. It has the typical form of a Fermi distribution with an effective temperature and chemical potential. The effective temperature and chemical potential in this low-energy term are determined by the intensity of carriers' generation, the speed of electron-phonon relaxation, rates ofmore » inter-band recombination, and electron capture on the defects. In addition, there is a substantial high-energy correction. This high-energy “tail” largely covers the conduction band. The shape of the high-energy “tail” strongly depends on the rate of electron-phonon relaxation but does not depend on the rates of recombination and trapping. We apply the theory to the calculation of a non-equilibrium distribution of electrons in an irradiated GaN. Probabilities of optical excitations from the valence to conduction band and electron-phonon coupling probabilities in GaN were calculated by the density functional perturbation theory. Our calculation of both parts of distribution function in gallium nitride shows that when the speed of the electron-phonon scattering is comparable with the rate of recombination and trapping then the contribution of the non-Fermi “tail” is comparable with that of the low-energy Fermi-like component. So the high-energy contribution can essentially affect the charge transport in the irradiated and highly doped semiconductors.« less

Direct optical state preparation of the dark exciton in a quantum dot

NASA Astrophysics Data System (ADS)

Lüker, S.; Kuhn, T.; Reiter, D. E.

2015-11-01

Because of their weak coupling to the electromagnetic field, dark excitons in semiconductor quantum dots possess extremely long lifetimes, which makes them attractive candidates for quantum information processing. On the other hand, the preparation and manipulation of dark states is challenging, because commonly used optical excitation mechanisms are not applicable. We propose an efficient mechanism for the deterministic preparation of the dark exciton exploiting the application of a tilted magnetic field and the optical excitation with a chirped, i.e., frequency modulated, laser pulse.

Low-loss electron energy loss spectroscopy: An atomic-resolution complement to optical spectroscopies and application to graphene

DOE PAGES

Kapetanakis, Myron; Zhou, Wu; Oxley, Mark P.; ...

2015-09-25

Photon-based spectroscopies have played a central role in exploring the electronic properties of crystalline solids and thin films. They are a powerful tool for probing the electronic properties of nanostructures, but they are limited by lack of spatial resolution. On the other hand, electron-based spectroscopies, e.g., electron energy loss spectroscopy (EELS), are now capable of subangstrom spatial resolution. Core-loss EELS, a spatially resolved analog of x-ray absorption, has been used extensively in the study of inhomogeneous complex systems. In this paper, we demonstrate that low-loss EELS in an aberration-corrected scanning transmission electron microscope, which probes low-energy excitations, combined with amore » theoretical framework for simulating and analyzing the spectra, is a powerful tool to probe low-energy electron excitations with atomic-scale resolution. The theoretical component of the method combines density functional theory–based calculations of the excitations with dynamical scattering theory for the electron beam. We apply the method to monolayer graphene in order to demonstrate that atomic-scale contrast is inherent in low-loss EELS even in a perfectly periodic structure. The method is a complement to optical spectroscopy as it probes transitions entailing momentum transfer. The theoretical analysis identifies the spatial and orbital origins of excitations, holding the promise of ultimately becoming a powerful probe of the structure and electronic properties of individual point and extended defects in both crystals and inhomogeneous complex nanostructures. The method can be extended to probe magnetic and vibrational properties with atomic resolution.« less

Aberration correction considering curved sample surface shape for non-contact two-photon excitation microscopy with spatial light modulator.

PubMed

Matsumoto, Naoya; Konno, Alu; Inoue, Takashi; Okazaki, Shigetoshi

2018-06-18

In this paper, excitation light wavefront modulation is performed considering the curved sample surface shape to demonstrate high-quality deep observation using two-photon excitation microscopy (TPM) with a dry objective lens. A large spherical aberration typically occurs when the refractive index (RI) interface between air and the sample is a plane perpendicular to the optical axis. Moreover, the curved sample surface shape and the RI mismatch cause various aberrations, including spherical ones. Consequently, the fluorescence intensity and resolution of the obtained image are degraded in the deep regions. To improve them, we designed a pre-distortion wavefront for correcting the aberration caused by the curved sample surface shape by using a novel, simple optical path length difference calculation method. The excitation light wavefront is modulated to the pre-distortion wavefront by a spatial light modulator incorporated in the TPM system before passing through the interface, where the RI mismatch occurs. Thus, the excitation light is condensed without aberrations. Blood vessels were thereby observed up to an optical depth of 2,000 μm in a cleared mouse brain by using a dry objective lens.

Eliminating Unwanted Far-Field Excitation in Objective-Type TIRF. Part I. Identifying Sources of Nonevanescent Excitation Light

PubMed Central

Brunstein, Maia; Teremetz, Maxime; Hérault, Karine; Tourain, Christophe; Oheim, Martin

2014-01-01

Total internal reflection fluorescence microscopy (TIRFM) achieves subdiffraction axial sectioning by confining fluorophore excitation to a thin layer close to the cell/substrate boundary. However, it is often unknown how thin this light sheet actually is. Particularly in objective-type TIRFM, large deviations from the exponential intensity decay expected for pure evanescence have been reported. Nonevanescent excitation light diminishes the optical sectioning effect, reduces contrast, and renders TIRFM-image quantification uncertain. To identify the sources of this unwanted fluorescence excitation in deeper sample layers, we here combine azimuthal and polar beam scanning (spinning TIRF), atomic force microscopy, and wavefront analysis of beams passing through the objective periphery. Using a variety of intracellular fluorescent labels as well as negative staining experiments to measure cell-induced scattering, we find that azimuthal beam spinning produces TIRFM images that more accurately portray the real fluorophore distribution, but these images are still hampered by far-field excitation. Furthermore, although clearly measureable, cell-induced scattering is not the dominant source of far-field excitation light in objective-type TIRF, at least for most types of weakly scattering cells. It is the microscope illumination optical path that produces a large cell- and beam-angle invariant stray excitation that is insensitive to beam scanning. This instrument-induced glare is produced far from the sample plane, inside the microscope illumination optical path. We identify stray reflections and high-numerical aperture aberrations of the TIRF objective as one important source. This work is accompanied by a companion paper (Pt.2/2). PMID:24606927

Carrier dynamics and the role of surface defects: Designing a photocatalyst for gas-phase CO 2 reduction

DOE PAGES

Hoch, Laura B.; Szymanski, Paul; Ghuman, Kulbir Kaur; ...

2016-11-28

In 2O 3-x(OH) y nanoparticles have been shown to function as an effective gas-phase photocatalyst for the reduction of CO 2 to CO via the reverse water–gas shift reaction. Their photocatalytic activity is strongly correlated to the number of oxygen vacancy and hydroxide defects present in the system. To better understand how such defects interact with photogenerated electrons and holes in these materials, we have studied the relaxation dynamics of In 2O 3-x(OH) y nanoparticles with varying concentration of defects using two different excitation energies corresponding to above-band-gap (318-nm) and near-band-gap (405-nm) excitations. Our results demonstrate that defects play amore » significant role in the excited-state, charge relaxation pathways. Higher defect concentrations result in longer excited-state lifetimes, which are attributed to improved charge separation. This correlates well with the observed trends in the photocatalytic activity. These results are further supported by density-functional theory calculations, which confirm the positions of oxygen vacancy and hydroxide defect states within the optical band gap of indium oxide. This enhanced understanding of the role these defects play in determining the optoelectronic properties and charge carrier dynamics can provide valuable insight toward the rational development of more efficient photocatalytic materials for CO 2 reduction.« less

Carrier dynamics and the role of surface defects: Designing a photocatalyst for gas-phase CO 2 reduction

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

Hoch, Laura B.; Szymanski, Paul; Ghuman, Kulbir Kaur

In 2O 3-x(OH) y nanoparticles have been shown to function as an effective gas-phase photocatalyst for the reduction of CO 2 to CO via the reverse water–gas shift reaction. Their photocatalytic activity is strongly correlated to the number of oxygen vacancy and hydroxide defects present in the system. To better understand how such defects interact with photogenerated electrons and holes in these materials, we have studied the relaxation dynamics of In 2O 3-x(OH) y nanoparticles with varying concentration of defects using two different excitation energies corresponding to above-band-gap (318-nm) and near-band-gap (405-nm) excitations. Our results demonstrate that defects play amore » significant role in the excited-state, charge relaxation pathways. Higher defect concentrations result in longer excited-state lifetimes, which are attributed to improved charge separation. This correlates well with the observed trends in the photocatalytic activity. These results are further supported by density-functional theory calculations, which confirm the positions of oxygen vacancy and hydroxide defect states within the optical band gap of indium oxide. This enhanced understanding of the role these defects play in determining the optoelectronic properties and charge carrier dynamics can provide valuable insight toward the rational development of more efficient photocatalytic materials for CO 2 reduction.« less

Excitation of resonances of microspheres on an optical fiber

NASA Astrophysics Data System (ADS)

Serpengüzel, A.; Arnold, S.; Griffel, G.

1995-04-01

Morphology-dependent resonances (MDR's) of solid microspheres are excited by using an optical fiber coupler. The narrowest measured MDR linewidths are limited by the excitation laser linewidth ( < 0.025 nm). Only MDR's, with an on-resonance to off-resonance intensity ratio of 104, contribute to scattering. The intensity of various resonance orders is understood by the localization principle and the recently developed generalized Lorentz-Mie theory. The microsphere fiber system has potential for becoming a building block in dispersive microphotonics. The basic physics underlying our approach may be considered a harbinger for the coupling of active photonic microstructures such as microdisk lasers.

Optical Bistability under Nonresonant Excitation in Spinor Polariton Condensates

NASA Astrophysics Data System (ADS)

Pickup, L.; Kalinin, K.; Askitopoulos, A.; Hatzopoulos, Z.; Savvidis, P. G.; Berloff, N. G.; Lagoudakis, P. G.

2018-06-01

We realize bistability in the spinor of polariton condensates under nonresonant optical excitation and in the absence of biasing external fields. Numerical modeling of the system using the Ginzburg-Landau equation with an internal Josephson coupling between the two spin components of the condensate qualitatively describes the experimental observations. We demonstrate that polariton spin bistability strongly depends on the condensate's overlap with the exciton reservoir by tuning the excitation geometry and sample temperature. We obtain noncollapsing bistability hysteresis loops for a record range of sweep times, [10 μ s , 1 s], offering a promising route to spin switches and spin memory elements.

Holonomic Quantum Control by Coherent Optical Excitation in Diamond.

PubMed

Zhou, Brian B; Jerger, Paul C; Shkolnikov, V O; Heremans, F Joseph; Burkard, Guido; Awschalom, David D

2017-10-06

Although geometric phases in quantum evolution are historically overlooked, their active control now stimulates strategies for constructing robust quantum technologies. Here, we demonstrate arbitrary single-qubit holonomic gates from a single cycle of nonadiabatic evolution, eliminating the need to concatenate two separate cycles. Our method varies the amplitude, phase, and detuning of a two-tone optical field to control the non-Abelian geometric phase acquired by a nitrogen-vacancy center in diamond over a coherent excitation cycle. We demonstrate the enhanced robustness of detuned gates to excited-state decoherence and provide insights for optimizing fast holonomic control in dissipative quantum systems.

Holonomic Quantum Control by Coherent Optical Excitation in Diamond

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

Zhou, Brian B.; Jerger, Paul C.; Shkolnikov, V. O.

Although geometric phases in quantum evolution are historically overlooked, their active control now stimulates strategies for constructing robust quantum technologies. Here, we demonstrate arbitrary singlequbit holonomic gates from a single cycle of nonadiabatic evolution, eliminating the need to concatenate two separate cycles. Our method varies the amplitude, phase, and detuning of a two-tone optical field to control the non-Abelian geometric phase acquired by a nitrogen-vacancy center in diamond over a coherent excitation cycle. We demonstrate the enhanced robustness of detuned gates to excited-state decoherence and provide insights for optimizing fast holonomic control in dissipative quantum systems.

Programmable light-controlled shape changes in layered polymer nanocomposites.

PubMed

Zhu, Zhichen; Senses, Erkan; Akcora, Pinar; Sukhishvili, Svetlana A

2012-04-24

We present soft, layered nanocomposites that exhibit controlled swelling anisotropy and spatially specific shape reconfigurations in response to light irradiation. The use of gold nanoparticles grafted with a temperature-responsive polymer (poly(N-isopropylacrylamide), PNIPAM) with layer-by-layer (LbL) assembly allowed placement of plasmonic structures within specific regions in the film, while exposure to light caused localized material deswelling by a photothermal mechanism. By layering PNIPAM-grafted gold nanoparticles in between nonresponsive polymer stacks, we have achieved zero Poisson's ratio materials that exhibit reversible, light-induced unidirectional shape changes. In addition, we report rheological properties of these LbL assemblies in their equilibrium swollen states. Moreover, incorporation of dissimilar plasmonic nanostructures (solid gold nanoparticles and nanoshells) within different material strata enabled controlled shrinkage of specific regions of hydrogels at specific excitation wavelengths. The approach is applicable to a wide range of metal nanoparticles and temperature-responsive polymers and affords many advanced build-in options useful in optically manipulated functional devices, including precise control of plasmonic layer thickness, tunability of shape variations to the excitation wavelength, and programmable spatial control of optical response.

Optical activity and electronic absorption spectra of some simple nucleosides related to cytidine and uridine: all-valence-shell molecular orbital calculations.

PubMed Central

Miles, D W; Redington, P K; Miles, D L; Eyring, H

1981-01-01

The circular dichroism and electronic absorption of three simple model systems for cytidine and uridine have been measured to 190 nm. The molecular spectral properties (excitation wavelengths, oscillator strengths, rotational strengths, and polarization directions) and electronic transitional patterns were investigated by using wave functions of the entire nucleoside with the goal of establishing the reliability of the theoretical method. The computed electronic absorption quantities were shown to be in satisfactory agreement with experimental data. It was found that the computed optical rotatory strengths of the B2u and E1u electronic transitions and lowest observed n-pi transition are in good agreement with experimental values. Electronic transitions were characterized by their electronic transitional patterns derived from population analysis of the transition density matrix. The theoretical rotational strengths associated with the B2u and E1u transitions stabilize after the use of just a few singly excited configurations in the configuration interaction basis and, hypothetically, are more reliable as indicators of conformation in pyrimidine nucleosides related to cytidine. PMID:6950393

Method for Estimating Bilirubin Isomerization Efficiency in Phototherapy to Treat Neonatal Jaundice

NASA Astrophysics Data System (ADS)

Lisenko, S. A.; Kugeiko, M. M.

2014-11-01

We propose a method for quantitative assessment of the efficacy of phototherapy to treat neonatal jaundice using the diffuse reflectance spectrum for the newborn's skin, based on the analytical dependence of the measured spectrum on the structural and morphological parameters of the skin, affecting the optical conditions in the medium, and an algorithm for rapid calculation of the bilirubin photoisomerization rate in the skin tissues as a function of the structural and morphological parameters of the skin and the wavelength of the exciting radiation. From the results of a numerical simulation of the process of radiation transport in the skin, we assess the stability of our method to variations in the scattering properties of the skin and the concentrations of its optically active chromophores (melanin, oxyhemoglobin, deoxyhemoglobin). We show that in order to achieve the maximum efficacy of phototherapy, we should use light from the range 484-496 nm. In this case, the intensity of the exciting radiation should be selected individually for each newborn according to the bilirubin photoisomerization rate characteristic for it.

Spectroscopic study of excitations in pi-conjugated polymers

NASA Astrophysics Data System (ADS)

Yang, Cungeng

This dissertation deals with spin-physics of photo excitations in pi-conjugated polymers. Optical and magneto-optical spectroscopies, including continuous wave and time-resolved photo-induced absorption, photoluminescence, electroluminescence, and their optically detected magnetic resonance, were used to study steady state and transient photogeneration, energy transfer, spin relaxation, and spin dependent recombination process in the time domain from tens of nanoseconds to tens of milliseconds in polymer materials including regio-random poly (3-hexyl-thiophene-2,5-diyl), regio-regular poly (3-hexyl-thiophene-2,5-diyl), poly (9,9-dioctyl-fluorenyl-2,7-diyl), poly (poly (2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylene vinylene) of various morphologies, and transition metal complex poly (Pt-quinoxene). Our studies provided the tools to clarify the physical pictures regarding two types of long-lived photoexcitations, namely polarons (both germinate polaron-pairs, and unpaired polarons) and triplet excitons, which are the major excitations in these exotic semiconductors in electrical and optical related applications. From measurements of transient fluorescence and transient fluorescence detected magnetic resonance we show that photogenerated geminate polaron pairs live up to hundreds of microseconds following laser pulsed excitation. This conclusion is in agreement with the delayed formation of triplet excitons that we measured by transient photoinduced absorption. It also agrees with the weak spin-lattice relaxation rate in polymers that we measured using the optically detected magnetic resonance dynamic in thin films and organic light emitting devices. Randomly captured nongeminate polaron pairs were shown to be the major source of optically detected magnetic resonance signal at steady, state. We found that the dynamics and magnitude of the signal depend on the spin-relaxation rate, generation rate and decay rate of the geminate pairs and nongeminate pairs. Importantly we found that the spin-relaxation rate depends weakly on temperature and strongly on coupled heavy atom orbital and magnetic momentum dipole induced by dopants or high intensity excitation. Also the polaron generation rate is excitation energy and nano-morphology dependent; whereas the polaron decay rate is morphology and spin dependent.

Optical Absorption and Emission Mechanisms of Single Defects in Hexagonal Boron Nitride

NASA Astrophysics Data System (ADS)

Jungwirth, Nicholas R.; Fuchs, Gregory D.

2017-08-01

We investigate the polarization selection rules of sharp zero-phonon lines (ZPLs) from isolated defects in hexagonal boron nitride (HBN) and compare our findings with the predictions of a Huang-Rhys model involving two electronic states. Our survey, which spans the spectral range ˜550 - 740 nm , reveals that, in disagreement with a two-level model, the absorption and emission dipoles are often misaligned. We relate the dipole misalignment angle (Δ θ ) of a ZPL to its energy shift from the excitation energy (Δ E ) and find that Δ θ ≈0 ° when Δ E corresponds to an allowed HBN phonon frequency and that 0 ° ≤Δ θ ≤90 ° when Δ E exceeds the maximum allowed HBN phonon frequency. Consequently, a two-level Huang-Rhys model succeeds at describing excitations mediated by the creation of one optical phonon but fails at describing excitations that require the creation of multiple phonons. We propose that direct excitations requiring the creation of multiple phonons are inefficient due to the low Huang-Rhys factors in HBN and that these ZPLs are instead excited indirectly via an intermediate electronic state. This hypothesis is corroborated by polarization measurements of an individual ZPL excited with two distinct wavelengths that indicate a single ZPL may be excited by multiple mechanisms. These findings provide new insight on the nature of the optical cycle of novel defect-based single-photon sources in HBN.

Graphene-on-silicon hybrid plasmonic-photonic integrated circuits.

PubMed

Xiao, Ting-Hui; Cheng, Zhenzhou; Goda, Keisuke

2017-06-16

Graphene surface plasmons (GSPs) have shown great potential in biochemical sensing, thermal imaging, and optoelectronics. To excite GSPs, several methods based on the near-field optical microscope and graphene nanostructures have been developed in the past few years. However, these methods suffer from their bulky setups and low GSP-excitation efficiency due to the short interaction length between free-space vertical excitation light and the atomic layer of graphene. Here we present a CMOS-compatible design of graphene-on-silicon hybrid plasmonic-photonic integrated circuits that achieve the in-plane excitation of GSP polaritons as well as localized surface plasmon (SP) resonance. By employing a suspended membrane slot waveguide, our design is able to excite GSP polaritons on a chip. Moreover, by utilizing a graphene nanoribbon array, we engineer the transmission spectrum of the waveguide by excitation of localized SP resonance. Our theoretical and computational study paves a new avenue to enable, modulate, and monitor GSPs on a chip, potentially applicable for the development of on-chip electro-optic devices.

Optimization of the excitation light sheet in selective plane illumination microscopy

PubMed Central

Gao, Liang

2015-01-01

Selective plane illumination microscopy (SPIM) allows rapid 3D live fluorescence imaging on biological specimens with high 3D spatial resolution, good optical sectioning capability and minimal photobleaching and phototoxic effect. SPIM gains its advantage by confining the excitation light near the detection focal plane, and its performance is determined by the ability to create a thin, large and uniform excitation light sheet. Several methods have been developed to create such an excitation light sheet for SPIM. However, each method has its own strengths and weaknesses, and tradeoffs must be made among different aspects in SPIM imaging. In this work, we present a strategy to select the excitation light sheet among the latest SPIM techniques, and to optimize its geometry based on spatial resolution, field of view, optical sectioning capability, and the sample to be imaged. Besides the light sheets discussed in this work, the proposed strategy is also applicable to estimate the SPIM performance using other excitation light sheets. PMID:25798312

Photoacoustic thermal flowmetry with a single light source

NASA Astrophysics Data System (ADS)

Liu, Wei; Lan, Bangxin; Hu, Leo; Chen, Ruimin; Zhou, Qifa; Yao, Junjie

2017-09-01

We report a photoacoustic thermal flowmetry based on optical-resolution photoacoustic microscopy (OR-PAM) using a single laser source for both thermal tagging and photoacoustic excitation. When an optically absorbing medium is flowing across the optical focal zone of OR-PAM, a small volume of the medium within the optical focus is repeatedly illuminated and heated by a train of laser pulses with a high repetition rate. The average temperature of the heated volume at each laser pulse is indicated by the photoacoustic signal excited by the same laser pulse due to the well-established linear relationship between the Grueneisen coefficient and the local temperature. The thermal dynamics of the heated medium volume, which are closely related to the flow speed, can therefore be measured from the time course of the detected photoacoustic signals. Here, we have developed a lumped mathematical model to describe the time course of the photoacoustic signals as a function of the medium's flow speed. We conclude that the rising time constant of the photoacoustic signals is linearly dependent on the flow speed. Thus, the flow speed can be quantified by fitting the measured photoacoustic signals using the derived mathematical model. We first performed proof-of-concept experiments using defibrinated bovine blood flowing in a plastic tube. The experiment results have demonstrated that the proposed method has high accuracy (˜±6%) and a wide range of measurable flow speeds. We further validated the method by measuring the blood flow speeds of the microvasculature in a mouse ear in vivo.

Integration of optically active Neodymium ions in Niobium devices (Nd:Nb): quantum memory for hybrid quantum entangled systems

NASA Astrophysics Data System (ADS)

Nayfeh, O. M.; Chao, D.; Djapic, N.; Sims, P.; Liu, B.; Sharma, S.; Lerum, L.; Fahem, M.; Dinh, V.; Zlatanovic, S.; Lynn, B.; Torres, C.; Higa, B.; Moore, J.; Upchurch, A.; Cothern, J.; Tukeman, M.; Barua, R.; Davidson, B.; Ramirez, A. D.; Rees, C. D.; Anant, V.; Kanter, G. S.

2017-08-01

Optically active rare-earth Neodymium (Nd) ions are integrated in Niobium (Nb) thin films forming a new quantum memory device (Nd:Nb) targeting long-lived coherence times and multi-functionality enabled by both spin and photon storage properties. Nb is implanted with Nd spanning 10-60 keV energy and 1013-1014 cm-2 dose producing a 1- 3% Nd:Nb concentration as confirmed by energy-dispersive X-ray spectroscopy. Scanning confocal photoluminescence (PL) at 785 nm excitation are made and sharp emission peaks from the 4F3/2 -< 4I11/2 Nd3+ transition at 1064-1070 nm are examined. In contrast, un-implanted Nb is void of any peaks. Line-shapes at room temperature are fit with Lorentzian profiles with line-widths of 4-5 nm and 1.3 THz bandwidth and the impacts of hyperfine splitting via the metallic crystal potential are apparent and the co-contribution of implant induced defects. With increasing Nd from 1% to 3%, there is a 0.3 nm red shift and increased broadening to a 4.8 nm linewidth. Nd:Nb is photoconductive and responds strongly to applied fields. Furthermore, optically detected magnetic resonance (ODMR) measurements are presented spanning near-infrared telecom band. The modulation of the emission intensity with magnetic field and microwave power by integration of these magnetic Kramer type Nd ions is quantified along with spin echoes under pulsed microwave π-π/2 excitation. A hybrid system architecture is proposed using spin and photon quantum information storage with the nuclear and electron states of the Nd3+ and neighboring Nb atoms that can couple qubit states to hyperfine 7/2 spin states of Nd:Nb and onto NIR optical levels excitable with entangled single photons, thus enabling implementation of computing and networking/internet protocols in a single platform.

Evaluation of optical excitation conditions for ruthenium complex for biosensor optodes

NASA Astrophysics Data System (ADS)

Pieper, Sean; Zhong, Zhong; Lear, Kevin L.; Reardon, Ken

2007-03-01

Development of a fiber optic biosensor incorporating genetically engineered enzymes which catalyze chlorinated ethenes in an oxygen-consuming reaction for in situ monitoring of groundwater contaminants motivates optimization of optode excitation conditions. These conditions affect the sensitivity, signal-to-noise, and optode service life impacting the quality of the overall biosensor. Optodes are generally comprised of a fluorophore conjugated with a polymer as a substrate cross linked at the distal end of a fiber optic. We investigate the excitation conditions of tris(4,7-diphenyl-1,10-phenanthroline) ruthenium(II) chloride (Ru(dpp)3) conjugated with poly(vinyl alcohol) (PVOH) as an optode. A reported advantage of Ru(dpp)3 is that it has no emission spectral shift occurring under varying chemical and environmental conditions. Photostability degradation due to photobleaching of Ru(dpp)3 with PVOH as a substrate is explored by varying the optical irradiance of the fluorophore containing optode. Other issues relating to practical implementation of Ru(dpp)3 as oxygen sensitive biosensors will be discussed.

Asymmetric noise sensitivity of pulse trains in an excitable microlaser with delayed optical feedback

NASA Astrophysics Data System (ADS)

Terrien, Soizic; Krauskopf, Bernd; Broderick, Neil G. R.; Andréoli, Louis; Selmi, Foued; Braive, Rémy; Beaudoin, Grégoire; Sagnes, Isabelle; Barbay, Sylvain

2017-10-01

A semiconductor micropillar laser with delayed optical feedback is considered. In the excitable regime, we show that a single optical perturbation can trigger a train of pulses that is sustained for a finite duration. The distribution of the pulse train duration exhibits an exponential behavior characteristic of a noise-induced process driven by uncorrelated white noise present in the system. The comparison of experimental observations with theoretical and numerical analysis of a minimal model yields excellent agreement. Importantly, the random switch-off process takes place between two attractors of different nature: an equilibrium and a periodic orbit. Our analysis shows that there is a small time window during which the pulsations are very sensitive to noise, and this explains the observed strong bias toward switch-off. These results raise the possibility of all optical control of the pulse train duration that may have an impact for practical applications in photonics and may also apply to the dynamics of other noise-driven excitable systems with delayed feedback.

Plasmonic excitation-assisted optical and electric enhancement in ultra-thin solar cells: the influence of nano-strip cross section

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

Sabaeian, Mohammad, E-mail: sabaiean@scu.ac.ir; Heydari, Mehdi; Ajamgard, Narges

The effects of Ag nano-strips with triangle, rectangular and trapezoid cross sections on the optical absorption, generation rate, and short-circuit current density of ultra-thin solar cells were investigated. By putting the nano-strips as a grating structure on the top of the solar cells, the waveguide, surface plasmon polariton (SPP), and localized surface plasmon (LSP) modes, which are excited with the assistance of nano-strips, were evaluated in TE and TM polarizations. The results show, firstly, the TM modes are more influential than TE modes in optical and electrical properties enhancement of solar cell, because of plasmonic excitations in TM mode. Secondly,more » the trapezoid nano-strips reveal noticeable impact on the optical absorption, generation rate, and short-circuit current density enhancement than triangle and rectangular ones. In particular, the absorption of long wavelengths which is a challenge in ultra-thin solar cells is significantly improved by using Ag trapezoid nano-strips.« less

Optical properties of alkali halide crystals from all-electron hybrid TD-DFT calculations

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

Webster, R., E-mail: ross.webster07@imperial.ac.uk; Harrison, N. M.; Bernasconi, L.

2015-06-07

We present a study of the electronic and optical properties of a series of alkali halide crystals AX, with A = Li, Na, K, Rb and X = F, Cl, Br based on a recent implementation of hybrid-exchange time-dependent density functional theory (TD-DFT) (TD-B3LYP) in the all-electron Gaussian basis set code CRYSTAL. We examine, in particular, the impact of basis set size and quality on the prediction of the optical gap and exciton binding energy. The formation of bound excitons by photoexcitation is observed in all the studied systems and this is shown to be correlated to specific features ofmore » the Hartree-Fock exchange component of the TD-DFT response kernel. All computed optical gaps and exciton binding energies are however markedly below estimated experimental and, where available, 2-particle Green’s function (GW-Bethe-Salpeter equation, GW-BSE) values. We attribute this reduced exciton binding to the incorrect asymptotics of the B3LYP exchange correlation ground state functional and of the TD-B3LYP response kernel, which lead to a large underestimation of the Coulomb interaction between the excited electron and hole wavefunctions. Considering LiF as an example, we correlate the asymptotic behaviour of the TD-B3LYP kernel to the fraction of Fock exchange admixed in the ground state functional c{sub HF} and show that there exists one value of c{sub HF} (∼0.32) that reproduces at least semi-quantitatively the optical gap of this material.« less

Pulse-Shaping-Based Nonlinear Microscopy: Development and Applications

NASA Astrophysics Data System (ADS)

Flynn, Daniel Christopher

The combination of optical microscopy and ultrafast spectroscopy make the spatial characterization of chemical kinetics on the femtosecond time scale possible. Commercially available octave-spanning Ti:Sapphire oscillators with sub-8 fs pulse durations can drive a multitude of nonlinear transitions across a significant portion of the visible spectrum with minimal average power. Unfortunately, dispersion from microscope objectives broadens pulse durations, decreases temporal resolution and lowers the peak intensities required for driving nonlinear transitions. In this dissertation, pulse shaping is used to compress laser pulses after the microscope objective. By using a binary genetic algorithm, pulse-shapes are designed to enable selective two-photon excitation. The pulse-shapes are demonstrated in two-photon fluorescence of live COS-7 cells expressing GFP-variants mAmetrine and tdTomato. The pulse-shaping approach is applied to a new multiphoton fluorescence resonance energy transfer (FRET) stoichiometry method that quantifies donor and acceptor molecules in complex, as well as the ratio of total donor to acceptor molecules. Compared to conventional multi-photon imaging techniques that require laser tuning or multiple laser systems to selectively excite individual fluorophores, the pulse-shaping approach offers rapid selective multifluorphore imaging at biologically relevant time scales. By splitting the laser beam into two beams and building a second pulse shaper, a pulse-shaping-based pump-probe microscope is developed. The technique offers multiple imaging modalities, such as excited state absorption (ESA), ground state bleach (GSB), and stimulated emission (SE), enhancing contrast of structures via their unique quantum pathways without the addition of contrast agents. Pulse-shaping based pump-probe microscopy is demonstrated for endogenous chemical-contrast imaging of red blood cells. In the second section of this dissertation, ultrafast spectroscopic techniques are used to characterize structure-function relationships of two-photon absorbing GFP-type probes and optical limiting materials. Fluorescence lifetimes of GFP-type probes are shown to depend on functional group substitution position, therefore, enabling the synthesis of designer probes for the possible study of conformation changes and aggregation in biological systems. Similarly, it is determined that small differences in the structure and dimensionality of organometallic macrocycles result in a diverse set of optical properties, which serves as a basis for the molecular level design of nonlinear optical materials.

On the nature of the solvated electron in ice Ih.

PubMed

de Koning, Maurice; Fazzio, Adalberto; da Silva, Antônio José Roque; Antonelli, Alex

2016-02-14

The water-solvated excess electron (EE) is a key chemical agent whose hallmark signature, its asymmetric optical absorption spectrum, continues to be a topic of debate. While nearly all investigation has focused on the liquid-water solvent, the fact that the crystalline-water solvated EE shows a very similar visible absorption pattern has remained largely unexplored. Here, we present spin-polarized density-functional theory calculations subject to periodic boundary conditions of the interplay between an EE and a number of intrinsic lattice defects in ice Ih. Our results show that the optical absorption signatures in the presence of three unsaturated hydrogen bonds (HB) are very similar to those observed experimentally. Its low-energy side can be attributed to transitions between the EE ground state and a single localized excited level, in a picture that is different from that for the liquid solvent, where this portion has been associated with hydrogen-like s → p excitations. The blue tail, on the other hand, relates to transitions between the EE ground state and delocalized excited states, which is in line with the bound-to-continuum transition interpretations for the EE in liquid water. Finally, we find that, depending on the number of dangling HBs participating in the EE trap, its charge density may spontaneously break the spin degeneracy through exchange interactions with the surrounding electrons, displaying the many-electron quantum nature of the EE problem in ice Ih.

Dynamics of shaping ultrashort optical dissipative solitary pulses in the actively mode-locked semiconductor laser with an external long-haul single-mode fiber cavity

NASA Astrophysics Data System (ADS)

Shcherbakov, Alexandre S.; Moreno Zarate, Pedro

2010-02-01

We describe the conditions of shaping regular trains of optical dissipative solitary pulses, excited by multi-pulse sequences of periodic modulating signals, in the actively mode-locked semiconductor laser heterostructure with an external long-haul single-mode silicon fiber exhibiting square-law dispersion, cubic Kerr nonlinearity, and linear optical losses. The presented model for the analysis includes three principal contributions associated with the modulated gain, optical losses, as well as linear and nonlinear phase shifts. In fact, the trains of optical dissipative solitary pulses appear within simultaneous presenting and a balance of mutually compensating interactions between the second-order dispersion and cubic-law Kerr nonlinearity as well as between active medium gain and linear optical losses in the combined cavity. Within such a model, a contribution of the nonlinear Ginzburg-Landau operator to shaping the parameters of optical dissipative solitary pulses is described via exploiting an approximate variational procedure involving the technique of trial functions. Finally, the results of the illustrating proof-of-principle experiments are briefly presented and discussed in terms of optical dissipative solitary pulses.

Persistence and Lifelong Fidelity of Phase Singularities in Optical Random Waves.

PubMed

De Angelis, L; Alpeggiani, F; Di Falco, A; Kuipers, L

2017-11-17

Phase singularities are locations where light is twisted like a corkscrew, with positive or negative topological charge depending on the twisting direction. Among the multitude of singularities arising in random wave fields, some can be found at the same location, but only when they exhibit opposite topological charge, which results in their mutual annihilation. New pairs can be created as well. With near-field experiments supported by theory and numerical simulations, we study the persistence and pairing statistics of phase singularities in random optical fields as a function of the excitation wavelength. We demonstrate how such entities can encrypt fundamental properties of the random fields in which they arise.

The role of optical rectification in the generation of terahertz radiation from GaBiAs

NASA Astrophysics Data System (ADS)

Radhanpura, K.; Hargreaves, S.; Lewis, R. A.; Henini, M.

2009-06-01

We report on a detailed study of the emission of terahertz-frequency electromagnetic radiation from layers of GaBiyAs1-y (0≤y<0.04) grown by molecular beam epitaxy on (311)B and (001) GaAs substrates. We measure two orthogonally polarized components of the terahertz radiation emitted under excitation by ultrashort near-infrared laser pulses in both transmission and reflection geometries as a function of the crystal rotation about its surface normal as well as the effect of in-plane magnetic field and pump fluence on the terahertz emission. We conclude that the principal mechanism for terahertz generation is via optical rectification rather than transient currents.

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.

Boron difluoride dibenzoylmethane derivatives: Electronic structure and luminescence

NASA Astrophysics Data System (ADS)

Tikhonov, Sergey A.; Vovna, Vitaliy I.; Osmushko, Ivan S.; Fedorenko, Elena V.; Mirochnik, Anatoliy G.

2018-01-01

Electronic structure and optical properties of boron difluoride dibenzoylmethanate and four of its derivatives have been studied by X-ray photoelectron spectroscopy, absorption and luminescence spectroscopy and quantum chemistry (DFT, TDDFT). The relative quantum luminescence yields have been revealed to correlate with charge transfers of HOMO-LUMO transitions, energy barriers of aromatic substituents rotation and the lifetime of excited states in the investigated complexes. The bathochromic shift of intensive bands in the optical spectra has been observed to occur when the functional groups are introduced into p-positions of phenyl cycles due to destabilizing HOMO levels. Calculated energy intervals between electronic levels correlate well with XPS spectra structure of valence and core electrons.

Persistence and Lifelong Fidelity of Phase Singularities in Optical Random Waves

NASA Astrophysics Data System (ADS)

De Angelis, L.; Alpeggiani, F.; Di Falco, A.; Kuipers, L.

2017-11-01

Phase singularities are locations where light is twisted like a corkscrew, with positive or negative topological charge depending on the twisting direction. Among the multitude of singularities arising in random wave fields, some can be found at the same location, but only when they exhibit opposite topological charge, which results in their mutual annihilation. New pairs can be created as well. With near-field experiments supported by theory and numerical simulations, we study the persistence and pairing statistics of phase singularities in random optical fields as a function of the excitation wavelength. We demonstrate how such entities can encrypt fundamental properties of the random fields in which they arise.

Optical feedback structures and methods of making

DOEpatents

None

2014-11-18

An optical resonator can include an optical feedback structure disposed on a substrate, and a composite including a matrix including a chromophore. The composite disposed on the substrate and in optical communication with the optical feedback structure. The chromophore can be a semiconductor nanocrystal. The resonator can provide laser emission when excited.

Size and shape dependence of electronic and optical excitations in TiO2 nanocrystals

NASA Astrophysics Data System (ADS)

Baishya, Kopinjol; Ogut, Serdar

2013-03-01

We present results for the electronic structures, quasi-particle gaps, and the absorption spectra of TiO2 nanocrystals of both rutile and anatase phases with various shapes, sizes, and surfaces exposed. We study the size and shape dependences of these electronic and optical properties, computed both within time-dependent density functional theory and many-body perturbation methods such as the GW-BSE, using appropriately passivated nanocrystals to mimic bulk termination. Surface effects are examined by using nanocrystals of various sizes with particular surfaces, such as (110) in rutile and (101) in anatase phases, exposed. We interpret the resulting optical absorption spectra of these nanocrystals in terms of the bulk spectra and compare them with predictions from classical Mie-Gans theory. This work was supported by the DOE Grant No. DE-FG02-09ER16072.

Deep donor state of the copper acceptor as a source of green luminescence in ZnO

NASA Astrophysics Data System (ADS)

Lyons, J. L.; Alkauskas, A.; Janotti, A.; Van de Walle, C. G.

2017-07-01

Copper impurities have long been linked with green luminescence (GL) in ZnO. Copper is known to introduce an acceptor level close to the conduction band of ZnO, and the GL has conventionally been attributed to transitions involving an excited state which localizes holes on neighboring oxygen atoms. To date, a theoretical description of the optical properties of such deep centers has been difficult to achieve due to the limitations of functionals in the density functional theory. Here, we employ a screened hybrid density functional to calculate the properties of Cu in ZnO. In agreement with the experiment, we find that CuZn features an acceptor level near the conduction band of ZnO. However, we find that CuZn also gives rise to a deep donor level 0.46 eV above the valence band of ZnO; the calculated optical transitions involving this state agree well with the GL observed in ZnO:Cu.

Quantum interference effects on the intensity of the G modes in double-walled carbon nanotubes

DOE PAGES

Tran, Huy Nam; Blancon, Jean-Christophe Robert; Arenal, Raul; ...

2017-05-08

The effects of quantum interferences on the excitation dependence of the intensity of G modes have been investigated on single-walled carbon nanotubes [Duque et al., Phys. Rev. Lett.108, 117404 (2012)]. In this work, by combining optical absorption spectroscopy and Raman scattering on individual index identified double-walled carbon nanotubes, we examine the experimental excitation dependence of the intensity of longitudinal optical and transverse optical G modes of the constituent inner and outer single-walled carbon nanotubes. The observed striking dependencies are understood in terms of quantum interference effects. Considering such effects, the excitation dependence of the different components of the G modesmore » permit to unambiguously assign each of them as originating from the longitudinal or transverse G modes of inner and outer tubes.« less

Quantum interference effects on the intensity of the G modes in double-walled carbon nanotubes

NASA Astrophysics Data System (ADS)

Tran, H. N.; Blancon, J.-C.; Arenal, R.; Parret, R.; Zahab, A. A.; Ayari, A.; Vallée, F.; Del Fatti, N.; Sauvajol, J.-L.; Paillet, M.

2017-05-01

The effects of quantum interferences on the excitation dependence of the intensity of G modes have been investigated on single-walled carbon nanotubes [Duque et al., Phys. Rev. Lett. 108, 117404 (2012), 10.1103/PhysRevLett.108.117404]. In this work, by combining optical absorption spectroscopy and Raman scattering on individual index identified double-walled carbon nanotubes, we examine the experimental excitation dependence of the intensity of longitudinal optical and transverse optical G modes of the constituent inner and outer single-walled carbon nanotubes. The observed striking dependencies are understood in terms of quantum interference effects. Considering such effects, the excitation dependence of the different components of the G modes permits us to unambiguously assign each of them as originating from the longitudinal or transverse G modes of inner and outer tubes.

Quantum interference effects on the intensity of the G modes in double-walled carbon nanotubes

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

Tran, Huy Nam; Blancon, Jean-Christophe Robert; Arenal, Raul

The effects of quantum interferences on the excitation dependence of the intensity of G modes have been investigated on single-walled carbon nanotubes [Duque et al., Phys. Rev. Lett.108, 117404 (2012)]. In this work, by combining optical absorption spectroscopy and Raman scattering on individual index identified double-walled carbon nanotubes, we examine the experimental excitation dependence of the intensity of longitudinal optical and transverse optical G modes of the constituent inner and outer single-walled carbon nanotubes. The observed striking dependencies are understood in terms of quantum interference effects. Considering such effects, the excitation dependence of the different components of the G modesmore » permit to unambiguously assign each of them as originating from the longitudinal or transverse G modes of inner and outer tubes.« less

Threshold singularities in a Fermi gas with attractive potential in one dimension

DOE PAGES

Schlottmann, P.; Zvyagin, A. A.

2015-01-15

We consider the one-dimensional gas of fermions with spin S interacting via an attractive δ-function potential using the Bethe Ansatz solution. In zero magnetic field the atoms form bound states of N=2S + 1 fermions, i.e. generalized Cooper states with each atom having a different spin component. For low energy excitations the system is a Luttinger liquid and is properly described by a conformal field theory with conformal charge c=1. The linear dispersion of a Luttinger liquid is asymptotically exact in the low-energy limit where the band curvature terms in the dispersion are irrelevant. For higher energy excitations, however, themore » spectral function displays deviations in the neighborhood of the single-particle (hole) energy, which can be described by an effective X-ray edge type model. Using the Bethe Ansatz solution we obtain expressions for the critical exponents for the single-particle (hole) Green’s function. This model can be relevant in the context of ultracold atoms with effective total spin S confined to an elongated optical trap.« less

Succinic acid functionalized silver nanoparticles (Suc-Ag NPs) for colorimetric sensing of melamine

NASA Astrophysics Data System (ADS)

Rajar, Kausar; Sirajuddin; Balouch, Aamna; Bhanger, M. I.; Shah, Muhammad Tariq; Shaikh, Tayyaba; Siddiqui, Samia

2018-03-01

In this study, a quantitative colorimetric sensing strategy is developed for the rapid, sensitive and selective determination of melamine. The sensing system relies on the application of succinic acid as a selective recognition probe functionalized over Ag NPs. The synthesized Ag NPs were modified with cysteamine to induce positively charged atmosphere which allowed easy and favorable functionalization of succinic acid. The di-carboxyl nature of succinic acid enabled its binding to both cysteamine and melamine. The strong and favorable linkage between succinic acids carbonyl and amine moieties of melamine triggered aggregation of silver NPs producing a significant shift in the measured absorption excitation. This change in the excitation along with the colorimetric response was found linearly proportional to the melamine concentration in the range of 0.1-1.2 μM. The developed sensor system is simple and unlike electrostatic attraction based sensor system utilize selective linkage for the recognition of melamine. In addition to this, the developed optical probe can efficiently be used for the determination of melamine in milk samples.

Exchange interaction between the triplet exciton and the localized spin in copper-phthalocyanine.

PubMed

Wu, Wei

2014-06-14

Triplet excitonic state in the organic molecule may arise from a singlet excitation and the following inter-system crossing. Especially for a spin-bearing molecule, an exchange interaction between the triplet exciton and the original spin on the molecule can be expected. In this paper, such exchange interaction in copper-phthalocyanine (CuPc, spin-½) was investigated from first-principles by using density-functional theory within a variety of approximations to the exchange correlation, ranging from local-density approximation to long-range corrected hybrid-exchange functional. The magnitude of the computed exchange interaction is in the order of meV with the minimum value (1.5 meV, ferromagnetic) given by the long-range corrected hybrid-exchange functional CAM-B3LYP. This exchange interaction can therefore give rise to a spin coherence with an oscillation period in the order of picoseconds, which is much shorter than the triplet lifetime in CuPc (typically tens of nanoseconds). This implies that it might be possible to manipulate the localized spin on Cu experimentally using optical excitation and inter-system crossing well before the triplet state disappears.

A surface-bound molecule that undergoes optically biased Brownian rotation.

PubMed

Hutchison, James A; Uji-i, Hiroshi; Deres, Ania; Vosch, Tom; Rocha, Susana; Müller, Sibylle; Bastian, Andreas A; Enderlein, Jörg; Nourouzi, Hassan; Li, Chen; Herrmann, Andreas; Müllen, Klaus; De Schryver, Frans; Hofkens, Johan

2014-02-01

Developing molecular systems with functions analogous to those of macroscopic machine components, such as rotors, gyroscopes and valves, is a long-standing goal of nanotechnology. However, macroscopic analogies go only so far in predicting function in nanoscale environments, where friction dominates over inertia. In some instances, ratchet mechanisms have been used to bias the ever-present random, thermally driven (Brownian) motion and drive molecular diffusion in desired directions. Here, we visualize the motions of surface-bound molecular rotors using defocused fluorescence imaging, and observe the transition from hindered to free Brownian rotation by tuning medium viscosity. We show that the otherwise random rotations can be biased by the polarization of the excitation light field, even though the associated optical torque is insufficient to overcome thermal fluctuations. The biased rotation is attributed instead to a fluctuating-friction mechanism in which photoexcitation of the rotor strongly inhibits its diffusion rate.