Broadband nonlinear optical response of monolayer MoSe2 under ultrafast excitation

NASA Astrophysics Data System (ADS)

Nie, Zhonghui; Trovatello, Chiara; Pogna, Eva A. A.; Dal Conte, Stefano; Miranda, Paulo B.; Kelleher, Edmund; Zhu, Chunhui; Turcu, Ion Crisitan Edmond; Xu, Yongbing; Liu, Kaihui; Cerullo, Giulio; Wang, Fengqiu

2018-01-01

Due to their strong light-matter interaction, monolayer transition metal dichalcogenides (TMDs) have proven to be promising candidates for nonlinear optics and optoelectronics. Here, we characterize the nonlinear absorption of chemical vapour deposition (CVD)-grown monolayer MoSe2 in the 720-810 nm wavelength range. Surprisingly, despite the presence of strong exciton resonances, monolayer MoSe2 exhibits a uniform modulation depth of ˜80 ± 3% and a saturation intensity of ˜2.5 ± 0.4 MW/cm2. In addition, pump-probe spectroscopy is performed to confirm the saturable absorption and reveal the photocarrier relaxation dynamics over hundreds of picoseconds. Our results unravel the unique broadband nonlinear absorptive behavior of monolayer MoSe2 under ultrafast excitation and highlight the potential of using monolayer TMDs as broadband ultrafast optical switches with customizable saturable absorption characteristics.

Parametric spectro-temporal analyzer (PASTA) for ultrafast optical performance monitoring

NASA Astrophysics Data System (ADS)

Zhang, Chi; Wong, Kenneth K. Y.

2013-12-01

Ultrafast optical spectrum monitoring is one of the most challenging tasks in observing ultrafast phenomena, such as the spectroscopy, dynamic observation of the laser cavity, and spectral encoded imaging systems. However, conventional method such as optical spectrum analyzer (OSA) spatially disperses the spectrum, but the space-to-time mapping is realized by mechanical rotation of a grating, so are incapable of operating at high speed. Besides the spatial dispersion, temporal dispersion provided by dispersive fiber can also stretches the spectrum in time domain in an ultrafast manner, but is primarily confined in measuring short pulses. In view of these constraints, here we present a real-time spectrum analyzer called parametric spectro-temporal analyzer (PASTA), which is based on the time-lens focusing mechanism. It achieves a 100-MHz frame rate and can measure arbitrary waveforms. For the first time, we observe the dynamic spectrum of an ultrafast swept-source: Fourier domain mode-locked (FDML) laser, and the spectrum evolution of a laser cavity during its stabilizing process. In addition to the basic single-lens structure, the multi-lens configurations (e.g. telescope or wide-angle scope) will provide a versatile operating condition, which can zoom in to achieve 0.05-nm resolution and zoom out to achieve 10-nm observation range, namely 17 times zoom in/out ratio. In view of the goal of achieving spectrum analysis with fine accuracy, PASTA provides a promising path to study the real-time spectrum of some dynamic phenomena and non-repetitive events, with orders of magnitude enhancement in the frame rate over conventional OSAs.

Ultrafast X-Ray Spectroscopy of Conical Intersections

NASA Astrophysics Data System (ADS)

Neville, Simon P.; Chergui, Majed; Stolow, Albert; Schuurman, Michael S.

2018-06-01

Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by general electronic degeneracies termed conical intersections, which play a key role, analogous to that of a transition state, in the electronic-nuclear dynamics of excited molecules. Using high-level ab initio quantum dynamics simulations, we studied time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) of the prototypical unsaturated organic chromophore, ethylene, following excitation to its S2(π π*) state. The TRXAS, in particular, is highly sensitive to all aspects of the ensuing dynamics. These x-ray spectroscopies provide a clear signature of the wave packet dynamics near conical intersections, related to charge localization effects driven by the nuclear dynamics. Given the ubiquity of charge localization in excited state dynamics, we believe that ultrafast x-ray spectroscopies offer a unique and powerful route to the direct observation of dynamics around conical intersections.

Pump-probe micro-spectroscopy by means of an ultra-fast acousto-optics delay line.

PubMed

Audier, Xavier; Balla, Naveen; Rigneault, Hervé

2017-01-15

We demonstrate femtosecond pump-probe transient absorption spectroscopy using a programmable dispersive filter as an ultra-fast delay line. Combined with fast synchronous detection, this delay line allows for recording of 6 ps decay traces at 34 kHz. With such acquisition speed, we perform single point pump-probe spectroscopy on bulk samples in 80 μs and hyperspectral pump-probe imaging over a field of view of 100 μm in less than a second. The usability of the method is illustrated in a showcase experiment to image and discriminate between two pigments in a mixture.

Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics

PubMed Central

Lejman, Mariusz; Vaudel, Gwenaelle; Infante, Ingrid C.; Chaban, Ievgeniia; Pezeril, Thomas; Edely, Mathieu; Nataf, Guillaume F.; Guennou, Mael; Kreisel, Jens; Gusev, Vitalyi E.; Dkhil, Brahim; Ruello, Pascal

2016-01-01

The ability to generate efficient giga–terahertz coherent acoustic phonons with femtosecond laser makes acousto-optics a promising candidate for ultrafast light processing, which faces electronic device limits intrinsic to complementary metal oxide semiconductor technology. Modern acousto-optic devices, including optical mode conversion process between ordinary and extraordinary light waves (and vice versa), remain limited to the megahertz range. Here, using coherent acoustic waves generated at tens of gigahertz frequency by a femtosecond laser pulse, we reveal the mode conversion process and show its efficiency in ferroelectric materials such as BiFeO3 and LiNbO3. Further to the experimental evidence, we provide a complete theoretical support to this all-optical ultrafast mechanism mediated by acousto-optic interaction. By allowing the manipulation of light polarization with gigahertz coherent acoustic phonons, our results provide a novel route for the development of next-generation photonic-based devices and highlight new capabilities in using ferroelectrics in modern photonics. PMID:27492493

Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics

NASA Astrophysics Data System (ADS)

Lejman, Mariusz; Vaudel, Gwenaelle; Infante, Ingrid C.; Chaban, Ievgeniia; Pezeril, Thomas; Edely, Mathieu; Nataf, Guillaume F.; Guennou, Mael; Kreisel, Jens; Gusev, Vitalyi E.; Dkhil, Brahim; Ruello, Pascal

2016-08-01

The ability to generate efficient giga-terahertz coherent acoustic phonons with femtosecond laser makes acousto-optics a promising candidate for ultrafast light processing, which faces electronic device limits intrinsic to complementary metal oxide semiconductor technology. Modern acousto-optic devices, including optical mode conversion process between ordinary and extraordinary light waves (and vice versa), remain limited to the megahertz range. Here, using coherent acoustic waves generated at tens of gigahertz frequency by a femtosecond laser pulse, we reveal the mode conversion process and show its efficiency in ferroelectric materials such as BiFeO3 and LiNbO3. Further to the experimental evidence, we provide a complete theoretical support to this all-optical ultrafast mechanism mediated by acousto-optic interaction. By allowing the manipulation of light polarization with gigahertz coherent acoustic phonons, our results provide a novel route for the development of next-generation photonic-based devices and highlight new capabilities in using ferroelectrics in modern photonics.

Interpreting Quasi-Thermal Effects in Ultrafast Spectroscopy of Hydrogen-Bonded Systems.

PubMed

Stingel, Ashley M; Petersen, Poul B

2018-03-15

Vibrational excitation of molecules in the condensed phase relaxes through vibrational modes of decreasing energy to ultimately generate an equilibrium state in which the energy is distributed among low-frequency modes. In ultrafast vibrational spectroscopy, changes in the vibrational features of hydrogen-bonded NH and OH stretch modes are typically observed to persist long after these high-frequency vibrations have relaxed. Due to the resemblance to the spectral changes caused by heating the sample, these features are typically described as arising from a hot ground state. However, these spectral features appear on ultrafast time scales that are much too fast to result from a true thermal state, and significant differences between the thermal difference spectrum and the induced quasi-thermal changes in ultrafast spectroscopy are often observed. Here, we examine and directly compare the thermal and quasi-thermal responses of the hydrogen-bonded homodimer of 7-azaindole with temperature-dependent FTIR spectroscopy and ultrafast mid-IR continuum spectroscopy. We find that the thermal difference spectra contain contributions from both dissociation of the hydrogen bonds and from frequency shifts due to changes in the thermal population of low-frequency modes. The transient spectra in ultrafast vibrational spectroscopy are also found to contain two contributions: initial frequency shifts over 2.3 ± 0.11 ps associated with equilibration of the initial excitation, and frequency shifts associated with the excitation of several fingerprint modes, which decay over 21.8 ± 0.11 ps, giving rise to a quasi-thermal response caused by a distribution of fingerprint modes being excited within the sample ensemble. This resembles the thermal frequency shifts due to population changes of low-frequency modes, but not the overall thermal spectrum, which is dominated by features caused by dimer dissociation. These findings provide insight into the changes in the vibrational spectrum

Modifying ultrafast optical response of sputtered VOX nanostructures in a broad spectral range by altering post annealing atmosphere

NASA Astrophysics Data System (ADS)

Kürüm, U.; Yaglioglu, H. G.; Küçüköz, B.; Oksuzoglu, R. M.; Yıldırım, M.; Yağcı, A. M.; Yavru, C.; Özgün, S.; Tıraş, T.; Elmali, A.

2015-01-01

Nanostructured VOX thin films were grown in a dc magnetron sputter system under two different Ar:O2 gas flow ratios. The films were annealed under vacuum and various ratios of O2/N2 atmospheres. The insulator-to-metal transition properties of the thin films were investigated by temperature dependent resistance measurement. Photo induced insulator-to-metal transition properties were investigated by Z-scan and ultrafast white light continuum pump probe spectroscopy measurements. Experiments showed that not only insulator-to-metal transition, but also wavelength dependence (from NIR to VIS) and time scale (from ns to ultrafast) of nonlinear optical response of the VOX thin films could be fine tuned by carefully adjusting post annealing atmosphere despite different initial oxygen content in the production. Fabricated VO2 thin films showed reflection change in the visible region due to photo induced phase transition. The results have general implications for easy and more effective fabrication of the nanostructured oxide systems with controllable electrical, optical, and ultrafast optical responses.

Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes

DOE PAGES

Seo, Minah; Yamaguchi, Hisato; Mohite, Aditya D.; ...

2016-02-15

We performed ultrafast optical microscopy on single flakes of atomically thin CVD-grown molybdenum disulfide, using non-degenerate femtosecond pump-probe spectroscopy to excite and probe carriers above and below the indirect and direct band gaps. These measurements reveal the influence of layer thickness on carrier dynamics when probing near the band gap. Furthermore, fluence-dependent measurements indicate that carrier relaxation is primarily influenced by surface-related defect and trap states after above-bandgap photoexcitation. Furthermore, the ability to probe femtosecond carrier dynamics in individual flakes can thus give much insight into light-matter interactions in these two-dimensional nanosystems.

Coherent multi-dimensional spectroscopy at optical frequencies in a single beam with optical readout

NASA Astrophysics Data System (ADS)

Seiler, Hélène; Palato, Samuel; Kambhampati, Patanjali

2017-09-01

Ultrafast coherent multi-dimensional spectroscopies form a powerful set of techniques to unravel complex processes, ranging from light-harvesting, chemical exchange in biological systems to many-body interactions in quantum-confined materials. Yet these spectroscopies remain complex to implement at the high frequencies of vibrational and electronic transitions, thereby limiting their widespread use. Here we demonstrate the feasibility of two-dimensional spectroscopy at optical frequencies in a single beam. Femtosecond optical pulses are spectrally broadened to a relevant bandwidth and subsequently shaped into phase coherent pulse trains. By suitably modulating the phases of the pulses within the beam, we show that it is possible to directly read out the relevant optical signals. This work shows that one needs neither complex beam geometries nor complex detection schemes in order to measure two-dimensional spectra at optical frequencies. Our setup provides not only a simplified experimental design over standard two-dimensional spectrometers but its optical readout also enables novel applications in microscopy.

PREFACE: Ultrafast biophotonics Ultrafast biophotonics

NASA Astrophysics Data System (ADS)

Gu, Min; Reid, Derryck; Ben-Yakar, Adela

2010-08-01

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

Room-temperature ultrafast nonlinear spectroscopy of a single molecule

NASA Astrophysics Data System (ADS)

Liebel, Matz; Toninelli, Costanza; van Hulst, Niek F.

2018-01-01

Single-molecule spectroscopy aims to unveil often hidden but potentially very important contributions of single entities to a system's ensemble response. Albeit contributing tremendously to our ever growing understanding of molecular processes, the fundamental question of temporal evolution, or change, has thus far been inaccessible, thus painting a static picture of a dynamic world. Here, we finally resolve this dilemma by performing ultrafast time-resolved transient spectroscopy on a single molecule. By tracing the femtosecond evolution of excited electronic state spectra of single molecules over hundreds of nanometres of bandwidth at room temperature, we reveal their nonlinear ultrafast response in an effective three-pulse scheme with fluorescence detection. A first excitation pulse is followed by a phase-locked de-excitation pulse pair, providing spectral encoding with 25 fs temporal resolution. This experimental realization of true single-molecule transient spectroscopy demonstrates that two-dimensional electronic spectroscopy of single molecules is experimentally within reach.

Ultralow-power and ultrafast all-optical tunable plasmon-induced transparency in metamaterials at optical communication range.

PubMed

Zhu, Yu; Hu, Xiaoyong; Fu, Yulan; Yang, Hong; Gong, Qihuang

2013-01-01

Actively all-optical tunable plasmon-induced transparency in metamaterials paves the way for achieving ultrahigh-speed quantum information processing chips. Unfortunately, up to now, very small experimental progress has been made for all-optical tunable plasmon-induced transparency in metamaterials in the visible and near-infrared range because of small third-order optical nonlinearity of conventional materials. The achieved operating pump intensity was as high as several GW/cm(2) order. Here, we report an ultralow-power and ultrafast all-optical tunable plasmon-induced transparency in metamaterials coated on polycrystalline indium-tin oxide layer at the optical communication range. Compared with previous reports, the threshold pump intensity is reduced by four orders of magnitude, while an ultrafast response time of picoseconds order is maintained. This work not only offers a way to constructing photonic materials with large nonlinearity and ultrafast response, but also opens up the possibility for realizing quantum solid chips and ultrafast integrated photonic devices based on metamaterials.

Ultralow-power and ultrafast all-optical tunable plasmon-induced transparency in metamaterials at optical communication range

PubMed Central

Zhu, Yu; Hu, Xiaoyong; Fu, Yulan; Yang, Hong; Gong, Qihuang

2013-01-01

Actively all-optical tunable plasmon-induced transparency in metamaterials paves the way for achieving ultrahigh-speed quantum information processing chips. Unfortunately, up to now, very small experimental progress has been made for all-optical tunable plasmon-induced transparency in metamaterials in the visible and near-infrared range because of small third-order optical nonlinearity of conventional materials. The achieved operating pump intensity was as high as several GW/cm2 order. Here, we report an ultralow-power and ultrafast all-optical tunable plasmon-induced transparency in metamaterials coated on polycrystalline indium-tin oxide layer at the optical communication range. Compared with previous reports, the threshold pump intensity is reduced by four orders of magnitude, while an ultrafast response time of picoseconds order is maintained. This work not only offers a way to constructing photonic materials with large nonlinearity and ultrafast response, but also opens up the possibility for realizing quantum solid chips and ultrafast integrated photonic devices based on metamaterials. PMID:23903825

Advanced optic fabrication using ultrafast laser radiation

NASA Astrophysics Data System (ADS)

Taylor, Lauren L.; Qiao, Jun; Qiao, Jie

2016-03-01

Advanced fabrication and finishing techniques are desired for freeform optics and integrated photonics. Methods including grinding, polishing and magnetorheological finishing used for final figuring and polishing of such optics are time consuming, expensive, and may be unsuitable for complex surface features while common photonics fabrication techniques often limit devices to planar geometries. Laser processing has been investigated as an alternative method for optic forming, surface polishing, structure writing, and welding, as direct tuning of laser parameters and flexible beam delivery are advantageous for complex freeform or photonics elements and material-specific processing. Continuous wave and pulsed laser radiation down to the nanosecond regime have been implemented to achieve nanoscale surface finishes through localized material melting, but the temporal extent of the laser-material interaction often results in the formation of a sub-surface heat affected zone. The temporal brevity of ultrafast laser radiation can allow for the direct vaporization of rough surface asperities with minimal melting, offering the potential for smooth, final surface quality with negligible heat affected material. High intensities achieved in focused ultrafast laser radiation can easily induce phase changes in the bulk of materials for processing applications. We have experimentally tested the effectiveness of ultrafast laser radiation as an alternative laser source for surface processing of monocrystalline silicon. Simulation of material heating associated with ultrafast laser-material interaction has been performed and used to investigate optimized processing parameters including repetition rate. The parameter optimization process and results of experimental processing will be presented.

Discrete decoding based ultrafast multidimensional nuclear magnetic resonance spectroscopy

NASA Astrophysics Data System (ADS)

Wei, Zhiliang; Lin, Liangjie; Ye, Qimiao; Li, Jing; Cai, Shuhui; Chen, Zhong

2015-07-01

The three-dimensional (3D) nuclear magnetic resonance (NMR) spectroscopy constitutes an important and powerful tool in analyzing chemical and biological systems. However, the abundant 3D information arrives at the expense of long acquisition times lasting hours or even days. Therefore, there has been a continuous interest in developing techniques to accelerate recordings of 3D NMR spectra, among which the ultrafast spatiotemporal encoding technique supplies impressive acquisition speed by compressing a multidimensional spectrum in a single scan. However, it tends to suffer from tradeoffs among spectral widths in different dimensions, which deteriorates in cases of NMR spectroscopy with more dimensions. In this study, the discrete decoding is proposed to liberate the ultrafast technique from tradeoffs among spectral widths in different dimensions by focusing decoding on signal-bearing sites. For verifying its feasibility and effectiveness, we utilized the method to generate two different types of 3D spectra. The proposed method is also applicable to cases with more than three dimensions, which, based on the experimental results, may widen applications of the ultrafast technique.

Recent advances in multidimensional ultrafast spectroscopy

NASA Astrophysics Data System (ADS)

Oliver, Thomas A. A.

2018-01-01

Multidimensional ultrafast spectroscopies are one of the premier tools to investigate condensed phase dynamics of biological, chemical and functional nanomaterial systems. As they reach maturity, the variety of frequency domains that can be explored has vastly increased, with experimental techniques capable of correlating excitation and emission frequencies from the terahertz through to the ultraviolet. Some of the most recent innovations also include extreme cross-peak spectroscopies that directly correlate the dynamics of electronic and vibrational states. This review article summarizes the key technological advances that have permitted these recent advances, and the insights gained from new multidimensional spectroscopic probes.

Recent advances in multidimensional ultrafast spectroscopy

PubMed Central

2018-01-01

Multidimensional ultrafast spectroscopies are one of the premier tools to investigate condensed phase dynamics of biological, chemical and functional nanomaterial systems. As they reach maturity, the variety of frequency domains that can be explored has vastly increased, with experimental techniques capable of correlating excitation and emission frequencies from the terahertz through to the ultraviolet. Some of the most recent innovations also include extreme cross-peak spectroscopies that directly correlate the dynamics of electronic and vibrational states. This review article summarizes the key technological advances that have permitted these recent advances, and the insights gained from new multidimensional spectroscopic probes. PMID:29410844

Carbon Nanotubes as an Ultrafast Emitter with a Narrow Energy Spread at Optical Frequency.

PubMed

Li, Chi; Zhou, Xu; Zhai, Feng; Li, Zhenjun; Yao, Fengrui; Qiao, Ruixi; Chen, Ke; Cole, Matthew Thomas; Yu, Dapeng; Sun, Zhipei; Liu, Kaihui; Dai, Qing

2017-08-01

Ultrafast electron pulses, combined with laser-pump and electron-probe technologies, allow ultrafast dynamics to be characterized in materials. However, the pursuit of simultaneous ultimate spatial and temporal resolution of microscopy and spectroscopy is largely subdued by the low monochromaticity of the electron pulses and their poor phase synchronization to the optical excitation pulses. Field-driven photoemission from metal tips provides high light-phase synchronization, but suffers large electron energy spreads (3-100 eV) as driven by a long wavelength laser (>800 nm). Here, ultrafast electron emission from carbon nanotubes (≈1 nm radius) excited by a 410 nm femtosecond laser is realized in the field-driven regime. In addition, the emitted electrons have great monochromaticity with energy spread as low as 0.25 eV. This great performance benefits from the extraordinarily high field enhancement and great stability of carbon nanotubes, superior to metal tips. The new nanotube-based ultrafast electron source opens exciting prospects for extending current characterization to sub-femtosecond temporal resolution as well as sub-nanometer spatial resolution. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultrafast electron transfer processes studied by pump-repump-probe spectroscopy.

PubMed

Fischer, Martin K; Gliserin, Alexander; Laubereau, Alfred; Iglev, Hristo

2011-03-01

The photodetachment of Br(-), I(-) and OH(-) in aqueous solution is studied by 2- and 3-pulse femtosecond spectroscopy. The UV excitation leads to fast electron separation followed by formation of a donor-electron pairs. An additional repump pulse is used for secondary excitation of the intermediates. The 3-pulse technique allows distinguishing the pair-intermediate from the fully separated electron. Using this method we observe a novel geminate recombination channel of .OH with adjacent hydrated electrons. The process leads to an ultrafast quenching (0.7 ps) of almost half the initial number of radicals. The phenomenon is not observed in Br(-) and I(-). Our results demonstrate the potential of the 3-pulse spectroscopy to elucidate the mechanism of ultrafast ET reactions. Photodetachment of aqueous anions studied by two- and three pulse spectroscopy. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Nonthermal ultrafast optical control of the magnetization in garnet films

NASA Astrophysics Data System (ADS)

Hansteen, Fredrik; Kimel, Alexey; Kirilyuk, Andrei; Rasing, Theo

2006-01-01

We demonstrate coherent optical control of the magnetization in ferrimagnetic garnet films on the femtosecond time scale through a combination of two different ultrafast and nonthermal photomagnetic effects and by employing multiple pump pulses. Linearly polarized laser pulses are shown to create a long-lived modification of the magnetocrystalline anisotropy via optically induced electron transfer between nonequivalent ion sites while circularly polarized pulses additionally act as strong transient magnetic field pulses originating from the nonabsorptive inverse Faraday effect. Due to the slow phonon-magnon interaction in these dielectrics, thermal effects of the laser excitation are clearly distinguished from the ultrafast nonthermal effects and can be seen only on the time scale of nanoseconds for sample temperatures near the Curie point. The reported effects open exciting possibilities for ultrafast manipulation of spins by light, and provide insight into the physics of magnetism on ultrafast time scales.

Localized, gradient-reversed ultrafast z-spectroscopy in vivo at 7T.

PubMed

Wilson, Neil E; D'Aquilla, Kevin; Debrosse, Catherine; Hariharan, Hari; Reddy, Ravinder

2016-10-01

To collect ultrafast z-spectra in vivo in situations where voxel homogeneity cannot be assured. Saturating in the presence of a gradient encodes the frequency offset spatially across a voxel. This encoding can be resolved by applying a similar gradient during readout. Acquiring additional scans with the gradient polarity reversed effectively mirrors the spatial locations of the frequency offsets so that the same physical location of a positive offset in the original scan will contribute a negative offset in the gradient-reversed scan. Gradient-reversed ultrafast z-spectroscopy (GRUFZS) was implemented and tested in a modified, localized PRESS sequence at 7T. Lysine phantoms were scanned at various concentrations and compared with coventionally-acquired z-spectra. Scans were acquired in vivo in human brain from homogeneous and inhomogeneous voxels with the ultrafast direction cycled between read, phase, and slice. Results were compared to those from a similar conventional z-spectroscopy PRESS-based sequence. Asymmetry spectra from GRUFZS are more consistent and reliable than those without gradient reversal and are comparable to those from conventional z-spectroscopy. GRUFZS offers significant acceleration in data acquisition compared to traditional chemical exchange saturation transfer methods with high spectral resolution and showed higher relative SNR effficiency. GRUFZS offers a method of collecting ultrafast z-spectra in voxels with the inhomogeneity often found in vivo. Magn Reson Med 76:1039-1046, 2016. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

Ultrafast photophysics of transition metal complexes.

PubMed

Chergui, Majed

2015-03-17

The properties of transition metal complexes are interesting not only for their potential applications in solar energy conversion, OLEDs, molecular electronics, biology, photochemistry, etc. but also for their fascinating photophysical properties that call for a rethinking of fundamental concepts. With the advent of ultrafast spectroscopy over 25 years ago and, more particularly, with improvements in the past 10-15 years, a new area of study was opened that has led to insightful observations of the intramolecular relaxation processes such as internal conversion (IC), intersystem crossing (ISC), and intramolecular vibrational redistribution (IVR). Indeed, ultrafast optical spectroscopic tools, such as fluorescence up-conversion, show that in many cases, intramolecular relaxation processes can be extremely fast and even shorter than time scales of vibrations. In addition, more and more examples are appearing showing that ultrafast ISC rates do not scale with the magnitude of the metal spin-orbit coupling constant, that is, that there is no heavy-atom effect on ultrafast time scales. It appears that the structural dynamics of the system and the density of states play a crucial role therein. While optical spectroscopy delivers an insightful picture of electronic relaxation processes involving valence orbitals, the photophysics of metal complexes involves excitations that may be centered on the metal (called metal-centered or MC) or the ligand (called ligand-centered or LC) or involve a transition from one to the other or vice versa (called MLCT or LMCT). These excitations call for an element-specific probe of the photophysics, which is achieved by X-ray absorption spectroscopy. In this case, transitions from core orbitals to valence orbitals or higher allow probing the electronic structure changes induced by the optical excitation of the valence orbitals, while also delivering information about the geometrical rearrangement of the neighbor atoms around the atom of

ULTRAFAST CHEMISTRY: Using Time-Resolved Vibrational Spectroscopy for Interrogation of Structural Dynamics

NASA Astrophysics Data System (ADS)

Nibbering, Erik T. J.; Fidder, Henk; Pines, Ehud

2005-05-01

Time-resolved infrared (IR) and Raman spectroscopy elucidates molecular structure evolution during ultrafast chemical reactions. Following vibrational marker modes in real time provides direct insight into the structural dynamics, as is evidenced in studies on intramolecular hydrogen transfer, bimolecular proton transfer, electron transfer, hydrogen bonding during solvation dynamics, bond fission in organometallic compounds and heme proteins, cis-trans isomerization in retinal proteins, and transformations in photochromic switch pairs. Femtosecond IR spectroscopy monitors the site-specific interactions in hydrogen bonds. Conversion between excited electronic states can be followed for intramolecular electron transfer by inspection of the fingerprint IR- or Raman-active vibrations in conjunction with quantum chemical calculations. Excess internal vibrational energy, generated either by optical excitation or by internal conversion from the electronic excited state to the ground state, is observable through transient frequency shifts of IR-active vibrations and through nonequilibrium populations as deduced by Raman resonances.

Chirped pulse digital holography for measuring the sequence of ultrafast optical wavefronts

NASA Astrophysics Data System (ADS)

Karasawa, Naoki

2018-04-01

Optical setups for measuring the sequence of ultrafast optical wavefronts using a chirped pulse as a reference wave in digital holography are proposed and analyzed. In this method, multiple ultrafast object pulses are used to probe the temporal evolution of ultrafast phenomena and they are interfered with a chirped reference wave to record a digital hologram. Wavefronts at different times can be reconstructed separately from the recorded hologram when the reference pulse can be treated as a quasi-monochromatic wave during the pulse width of each object pulse. The feasibility of this method is demonstrated by numerical simulation.

Time-resolved single-shot terahertz time-domain spectroscopy for ultrafast irreversible processes

NASA Astrophysics Data System (ADS)

Zhai, Zhao-Hui; Zhong, Sen-Cheng; Li, Jun; Zhu, Li-Guo; Meng, Kun; Li, Jiang; Liu, Qiao; Peng, Qi-Xian; Li, Ze-Ren; Zhao, Jian-Heng

2016-09-01

Pulsed terahertz spectroscopy is suitable for spectroscopic diagnostics of ultrafast events. However, the study of irreversible or single shot ultrafast events requires ability to record transient properties at multiple time delays, i.e., time resolved at single shot level, which is not available currently. Here by angular multiplexing use of femtosecond laser pulses, we developed and demonstrated a time resolved, transient terahertz time domain spectroscopy technique, where burst mode THz pulses were generated and then detected in a single shot measurement manner. The burst mode THz pulses contain 2 sub-THz pulses, and the time gap between them is adjustable up to 1 ns with picosecond accuracy, thus it can be used to probe the single shot event at two different time delays. The system can detect the sub-THz pulses at 0.1 THz-2.5 THz range with signal to noise ratio (SNR) of ˜400 and spectrum resolution of 0.05 THz. System design was described here, and optimizations of single shot measurement of THz pulses were discussed in detail. Methods to improve SNR were also discussed in detail. A system application was demonstrated where pulsed THz signals at different time delays of the ultrafast process were successfully acquired within single shot measurement. This time resolved transient terahertz time domain spectroscopy technique provides a new diagnostic tool for irreversible or single shot ultrafast events where dynamic information can be extracted at terahertz range within one-shot experiment.

Time-resolved single-shot terahertz time-domain spectroscopy for ultrafast irreversible processes.

PubMed

Zhai, Zhao-Hui; Zhong, Sen-Cheng; Li, Jun; Zhu, Li-Guo; Meng, Kun; Li, Jiang; Liu, Qiao; Peng, Qi-Xian; Li, Ze-Ren; Zhao, Jian-Heng

2016-09-01

Pulsed terahertz spectroscopy is suitable for spectroscopic diagnostics of ultrafast events. However, the study of irreversible or single shot ultrafast events requires ability to record transient properties at multiple time delays, i.e., time resolved at single shot level, which is not available currently. Here by angular multiplexing use of femtosecond laser pulses, we developed and demonstrated a time resolved, transient terahertz time domain spectroscopy technique, where burst mode THz pulses were generated and then detected in a single shot measurement manner. The burst mode THz pulses contain 2 sub-THz pulses, and the time gap between them is adjustable up to 1 ns with picosecond accuracy, thus it can be used to probe the single shot event at two different time delays. The system can detect the sub-THz pulses at 0.1 THz-2.5 THz range with signal to noise ratio (SNR) of ∼400 and spectrum resolution of 0.05 THz. System design was described here, and optimizations of single shot measurement of THz pulses were discussed in detail. Methods to improve SNR were also discussed in detail. A system application was demonstrated where pulsed THz signals at different time delays of the ultrafast process were successfully acquired within single shot measurement. This time resolved transient terahertz time domain spectroscopy technique provides a new diagnostic tool for irreversible or single shot ultrafast events where dynamic information can be extracted at terahertz range within one-shot experiment.

Ultrafast structural molecular dynamics investigated with 2D infrared spectroscopy methods.

PubMed

Kraack, Jan Philip

2017-10-25

Ultrafast, multi-dimensional infrared (IR) spectroscopy has been advanced in recent years to a versatile analytical tool with a broad range of applications to elucidate molecular structure on ultrafast timescales, and it can be used for samples in a many different environments. Following a short and general introduction on the benefits of 2D IR spectroscopy, the first part of this chapter contains a brief discussion on basic descriptions and conceptual considerations of 2D IR spectroscopy. Outstanding classical applications of 2D IR are used afterwards to highlight the strengths and basic applicability of the method. This includes the identification of vibrational coupling in molecules, characterization of spectral diffusion dynamics, chemical exchange of chemical bond formation and breaking, as well as dynamics of intra- and intermolecular energy transfer for molecules in bulk solution and thin films. In the second part, several important, recently developed variants and new applications of 2D IR spectroscopy are introduced. These methods focus on (i) applications to molecules under two- and three-dimensional confinement, (ii) the combination of 2D IR with electrochemistry, (iii) ultrafast 2D IR in conjunction with diffraction-limited microscopy, (iv) several variants of non-equilibrium 2D IR spectroscopy such as transient 2D IR and 3D IR, and (v) extensions of the pump and probe spectral regions for multi-dimensional vibrational spectroscopy towards mixed vibrational-electronic spectroscopies. In light of these examples, the important open scientific and conceptual questions with regard to intra- and intermolecular dynamics are highlighted. Such questions can be tackled with the existing arsenal of experimental variants of 2D IR spectroscopy to promote the understanding of fundamentally new aspects in chemistry, biology and materials science. The final part of the chapter introduces several concepts of currently performed technical developments, which aim at

Modelling multi-pulse population dynamics from ultrafast spectroscopy.

PubMed

van Wilderen, Luuk J G W; Lincoln, Craig N; van Thor, Jasper J

2011-03-21

Current advanced laser, optics and electronics technology allows sensitive recording of molecular dynamics, from single resonance to multi-colour and multi-pulse experiments. Extracting the occurring (bio-) physical relevant pathways via global analysis of experimental data requires a systematic investigation of connectivity schemes. Here we present a Matlab-based toolbox for this purpose. The toolbox has a graphical user interface which facilitates the application of different reaction models to the data to generate the coupled differential equations. Any time-dependent dataset can be analysed to extract time-independent correlations of the observables by using gradient or direct search methods. Specific capabilities (i.e. chirp and instrument response function) for the analysis of ultrafast pump-probe spectroscopic data are included. The inclusion of an extra pulse that interacts with a transient phase can help to disentangle complex interdependent pathways. The modelling of pathways is therefore extended by new theory (which is included in the toolbox) that describes the finite bleach (orientation) effect of single and multiple intense polarised femtosecond pulses on an ensemble of randomly oriented particles in the presence of population decay. For instance, the generally assumed flat-top multimode beam profile is adapted to a more realistic Gaussian shape, exposing the need for several corrections for accurate anisotropy measurements. In addition, the (selective) excitation (photoselection) and anisotropy of populations that interact with single or multiple intense polarised laser pulses is demonstrated as function of power density and beam profile. Using example values of real world experiments it is calculated to what extent this effectively orients the ensemble of particles. Finally, the implementation includes the interaction with multiple pulses in addition to depth averaging in optically dense samples. In summary, we show that mathematical modelling is

Modelling Multi-Pulse Population Dynamics from Ultrafast Spectroscopy

PubMed Central

van Wilderen, Luuk J. G. W.; Lincoln, Craig N.; van Thor, Jasper J.

2011-01-01

Current advanced laser, optics and electronics technology allows sensitive recording of molecular dynamics, from single resonance to multi-colour and multi-pulse experiments. Extracting the occurring (bio-) physical relevant pathways via global analysis of experimental data requires a systematic investigation of connectivity schemes. Here we present a Matlab-based toolbox for this purpose. The toolbox has a graphical user interface which facilitates the application of different reaction models to the data to generate the coupled differential equations. Any time-dependent dataset can be analysed to extract time-independent correlations of the observables by using gradient or direct search methods. Specific capabilities (i.e. chirp and instrument response function) for the analysis of ultrafast pump-probe spectroscopic data are included. The inclusion of an extra pulse that interacts with a transient phase can help to disentangle complex interdependent pathways. The modelling of pathways is therefore extended by new theory (which is included in the toolbox) that describes the finite bleach (orientation) effect of single and multiple intense polarised femtosecond pulses on an ensemble of randomly oriented particles in the presence of population decay. For instance, the generally assumed flat-top multimode beam profile is adapted to a more realistic Gaussian shape, exposing the need for several corrections for accurate anisotropy measurements. In addition, the (selective) excitation (photoselection) and anisotropy of populations that interact with single or multiple intense polarised laser pulses is demonstrated as function of power density and beam profile. Using example values of real world experiments it is calculated to what extent this effectively orients the ensemble of particles. Finally, the implementation includes the interaction with multiple pulses in addition to depth averaging in optically dense samples. In summary, we show that mathematical modelling is

UCEPR: Ultrafast localized CEST-spectroscopy with PRESS in phantoms and in vivo.

PubMed

Liu, Zheng; Dimitrov, Ivan E; Lenkinski, Robert E; Hajibeigi, Asghar; Vinogradov, Elena

2016-05-01

Chemical exchange saturation transfer (CEST) is a contrast mechanism enhancing low-concentration molecules through saturation transfer from their exchangeable protons to bulk water. Often many scans are acquired to form a Z-spectrum, making the CEST method time-consuming. Here, an ultrafast localized CEST-spectroscopy with PRESS (UCEPR) is proposed to obtain the entire Z-spectrum of a voxel using only two scans, significantly accelerating CEST. The approach combines ultrafast nonlocalized CEST spectroscopy with localization using PRESS. A field gradient is applied concurrently with the saturation pulse producing simultaneous saturation of all Z-spectrum frequencies that are also spatially encoded. A readout gradient during data acquisition resolves the spatial dependence of the CEST responses into frequency. UCEPR was tested on a 3T scanner both in phantoms and in vivo. In phantoms, a fast Z-spectroscopy acquisition of multiple pH-variant iopamidol samples was achieved with four- to seven-fold acceleration as compared to the conventional CEST methods. In vivo, amide proton transfer (APT) in white matter of healthy human brain was measured rapidly in 48 s and with high frequency resolution (≤ 0.2 ppm). Compared with conventional CEST methods, UCEPR has the advantage of rapidly acquiring high-resolution Z-spectra. Potential in vivo applications include ultrafast localized Z-spectroscopy, quantitative, or dynamic CEST studies. © 2015 Wiley Periodicals, Inc.

Coherent Femtosecond Spectroscopy and Nonlinear Optical Imaging on the Nanoscale

NASA Astrophysics Data System (ADS)

Kravtsov, Vasily

Optical properties of many materials and macroscopic systems are defined by ultrafast dynamics of electronic, vibrational, and spin excitations localized on the nanoscale. Harnessing these excitations for material engineering, optical computing, and control of chemical reactions has been a long-standing goal in science and technology. However, it is challenging due to the lack of spectroscopic techniques that can resolve processes simultaneously on the nanometer spatial and femtosecond temporal scales. This thesis describes the fundamental principles, implementation, and experimental demonstration of a novel type of ultrafast microscopy based on the concept of adiabatic plasmonic nanofocusing. Simultaneous spatio-temporal resolution on a nanometer-femtosecond scale is achieved by using a near-field nonlinear optical response induced by ultrafast surface plasmon polaritons nanofocused on a metal tip. First, we study the surface plasmon response in metallic structures and evaluate its prospects and limitations for ultrafast near-field microscopy. Through plasmon emission-based spectroscopy, we investigate dephasing times and interplay between radiative and non-radiative decay rates of localized plasmons and their modification due to coupling. We identify a new regime of quantum plasmonic coupling, which limits the achievable spatial resolution to several angstroms but at the same time provides a potential channel for generating ultrafast electron currents at optical frequencies. Next, we study propagation of femtosecond wavepackets of surface plasmon polaritons on a metal tip. In time-domain interferometric measurements we detect group delays that correspond to slowing of the plasmon polaritons down to 20% of the speed of light at the tip apex. This provides direct experimental verification of the plasmonic nanofocusing mechanism and suggests enhanced nonlinear optical interactions at the tip apex. We then measure a plasmon-generated third-order nonlinear optical

Ultrafast dynamics of electrons in ammonia.

PubMed

Vöhringer, Peter

2015-04-01

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

Photon-assisted electron energy loss spectroscopy and ultrafast imaging.

PubMed

Howie, Archie

2009-08-01

A variety of ways is described in which photons can be used not only for ultrafast electron microscopy but also to enormously widen the energy range of spatially-resolved electron spectroscopy. Periodic chains of femtosecond laser pulses are a particularly important and accurately timed source for single-shot imaging and diffraction as well as for several forms of pump-probe microscopy at even higher spatial resolution and sub-picosecond timing. Many exciting new fields are opened up for study by these developments. Ultrafast, single shot diffraction with intense pulses of X-rays supplemented by phase retrieval techniques may eventually offer a challenging alternative and purely photon-based route to dynamic imaging at high spatial resolution.

Ultrafast magnetodynamics with free-electron lasers

NASA Astrophysics Data System (ADS)

Malvestuto, Marco; Ciprian, Roberta; Caretta, Antonio; Casarin, Barbara; Parmigiani, Fulvio

2018-02-01

The study of ultrafast magnetodynamics has entered a new era thanks to the groundbreaking technological advances in free-electron laser (FEL) light sources. The advent of these light sources has made possible unprecedented experimental schemes for time-resolved x-ray magneto-optic spectroscopies, which are now paving the road for exploring the ultimate limits of out-of-equilibrium magnetic phenomena. In particular, these studies will provide insights into elementary mechanisms governing spin and orbital dynamics, therefore contributing to the development of ultrafast devices for relevant magnetic technologies. This topical review focuses on recent advancement in the study of non-equilibrium magnetic phenomena from the perspective of time-resolved extreme ultra violet (EUV) and soft x-ray spectroscopies at FELs with highlights of some important experimental results.

Apparatus and method for characterizing ultrafast polarization varying optical pulses

DOEpatents

Smirl, Arthur; Trebino, Rick P.

1999-08-10

Practical techniques are described for characterizing ultrafast potentially ultraweak, ultrashort optical pulses. The techniques are particularly suited to the measurement of signals from nonlinear optical materials characterization experiments, whose signals are generally too weak for full characterization using conventional techniques.

Fusion of Ultraviolet-Visible and Infrared Transient Absorption Spectroscopy Data to Model Ultrafast Photoisomerization.

PubMed

Debus, Bruno; Orio, Maylis; Rehault, Julien; Burdzinski, Gotard; Ruckebusch, Cyril; Sliwa, Michel

2017-08-03

Ultrafast photoisomerization reactions generally start at a higher excited state with excess of internal vibrational energy and occur via conical intersections. This leads to ultrafast dynamics which are difficult to investigate with a single transient absorption spectroscopy technique, be it in the ultraviolet-visible (UV-vis) or infrared (IR) domain. On one hand, the information available in the UV-vis domain is limited as only slight spectral changes are observed for different isomers. On the other hand, the interpretation of vibrational spectra is strongly hindered by intramolecular relaxation and vibrational cooling. These limitations can be circumvented by fusing UV-vis and IR transient absorption spectroscopy data in a multiset multivariate curve resolution analysis. We apply this approach to describe the spectrodynamics of the ultrafast cis-trans photoisomerization around the C-N double bond observed for aromatic Schiff bases. Twisted intermediate states could be elucidated, and isomerization was shown to occur through a continuous complete rotation. More broadly, data fusion can be used to rationalize a vast range of ultrafast photoisomerization processes of interest in photochemistry.

Ultrafast all-optical control of the magnetization in magnetic dielectrics

NASA Astrophysics Data System (ADS)

Kirilyuk, Andrei; Kimel, Alexey; Hansteen, Fredrik; Rasing, Theo; Pisarev, Roman V.

2006-08-01

The purpose of this review is to summarize the recent progress on laser-induced magnetization dynamics in magnetic dielectrics. Due to the slow phonon-magnon interaction in these materials, direct thermal effects of the laser excitation can only be seen on the time scale of almost a nanosecond and thus are clearly distinguished from the ultrafast nonthermal effects. However, laser pulses are shown to indirectly modify the magnetic anisotropy in rare-earth orthoferrites via the crystal field, and to bring about spin reorientation within a few picoseconds. More interesting, however, are the direct nonthermal effects of light on spin systems. We demonstrate coherent optical control of the magnetization in ferrimagnetic garnet films on a femtosecond time scale through a combination of two different ultrafast and nonthermal photomagnetic effects and by employing multiple pump pulses. Linearly polarized laser pulses are shown to create a long-lived modification of the magnetocrystalline anisotropy via optically induced electron transfer between nonequivalent ion sites. In addition, circularly polarized pulses are shown to act as strong transient magnetic field pulses originating from the nonabsorptive inverse Faraday effect. An all-optical scheme of excitation and detection of different antiferromagnetic resonance modes with frequencies of up to 500GHz will be discussed as well. The reported effects open new and exciting possibilities for ultrafast manipulation of spins by light and provide new insight into the physics of magnetism on ultrafast time scales.

Ultrafast all-optical technologies for bidirectional optical wireless communications.

PubMed

Jin, Xian; Hristovski, Blago A; Collier, Christopher M; Geoffroy-Gagnon, Simon; Born, Brandon; Holzman, Jonathan F

2015-04-01

In this Letter, a spherical retro-modulator architecture is introduced for operation as a bidirectional transceiver in passive optical wireless communication links. The architecture uses spherical retroreflection to enable retroreflection with broad directionality (2π steradians), and it uses all-optical beam interaction to enable modulation on ultrafast timescales (120 fs duration). The spherical retro-modulator is investigated from a theoretical standpoint and is fabricated for testing with three glasses, N-BK7, N-LASF9, and S-LAH79. It is found that the S-LAH79 structure provides the optimal refraction and nonlinearity for the desired retroreflection and modulation capabilities.

Ultrafast All-Optical Switching of Germanium-Based Flexible Metaphotonic Devices.

PubMed

Lim, Wen Xiang; Manjappa, Manukumara; Srivastava, Yogesh Kumar; Cong, Longqing; Kumar, Abhishek; MacDonald, Kevin F; Singh, Ranjan

2018-03-01

Incorporating semiconductors as active media into metamaterials offers opportunities for a wide range of dynamically switchable/tunable, technologically relevant optical functionalities enabled by strong, resonant light-matter interactions within the semiconductor. Here, a germanium-thin-film-based flexible metaphotonic device for ultrafast optical switching of terahertz radiation is experimentally demonstrated. A resonant transmission modulation depth of 90% is achieved, with an ultrafast full recovery time of 17 ps. An observed sub-picosecond decay constant of 670 fs is attributed to the presence of trap-assisted recombination sites in the thermally evaporated germanium film. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Apparatus and method for characterizing ultrafast polarization varying optical pulses

DOEpatents

Smirl, A.; Trebino, R.P.

1999-08-10

Practical techniques are described for characterizing ultrafast potentially ultraweak, ultrashort optical pulses. The techniques are particularly suited to the measurement of signals from nonlinear optical materials characterization experiments, whose signals are generally too weak for full characterization using conventional techniques. 2 figs.

Terahertz Spectroscopy of Low-Dimensional Nanomaterials: Nonlinear Emission and Ultrafast Electrodynamics

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

Luo, Liang; Wang, Jigang

Nonlinear and non-equilibrium properties of low-dimensional quantum materials are fundamental in nanoscale science yet transformative in nonlinear imaging/photonic technology today. These have been poorly addressed in many nano-materials despite of their well-established equilibrium optical and transport properties. The development of ultrafast terahertz (THz) sources and nonlinear spectroscopy tools facilitates understanding these issues and reveals a wide range of novel nonlinear and quantum phenomena that are not expected in bulk solids or atoms. In this paper, we discuss our recent discoveries in two model photonic and electronic nanostructures to solve two outstanding questions: (1) how to create nonlinear broadband terahertz emittersmore » using deeply subwavelength nanoscale meta-atom resonators? (2) How to access one-dimensional (1D) dark excitons and their non-equilibrium correlated states in single-walled carbon nanotubes (SWMTs)?« less

Terahertz Spectroscopy of Low-Dimensional Nanomaterials: Nonlinear Emission and Ultrafast Electrodynamics

DOE PAGES

Luo, Liang; Wang, Jigang

2016-01-01

Nonlinear and non-equilibrium properties of low-dimensional quantum materials are fundamental in nanoscale science yet transformative in nonlinear imaging/photonic technology today. These have been poorly addressed in many nano-materials despite of their well-established equilibrium optical and transport properties. The development of ultrafast terahertz (THz) sources and nonlinear spectroscopy tools facilitates understanding these issues and reveals a wide range of novel nonlinear and quantum phenomena that are not expected in bulk solids or atoms. In this paper, we discuss our recent discoveries in two model photonic and electronic nanostructures to solve two outstanding questions: (1) how to create nonlinear broadband terahertz emittersmore » using deeply subwavelength nanoscale meta-atom resonators? (2) How to access one-dimensional (1D) dark excitons and their non-equilibrium correlated states in single-walled carbon nanotubes (SWMTs)?« less

Population branching in the conical intersection of the retinal chromophore revealed by multipulse ultrafast optical spectroscopy.

PubMed

Zgrablić, Goran; Novello, Anna Maria; Parmigiani, Fulvio

2012-01-18

The branching ratio of the excited-state population at the conical intersection between the S(1) and S(0) energy surfaces (Φ(CI)) of a protonated Schiff base of all-trans retinal in protic and aprotic solvents was studied by multipulse ultrafast transient absorption spectroscopy. In particular, pump-dump-probe experiments allowed to isolate the S(1) reactive state and to measure the photoisomerization time constant with unprecedented precision. Starting from these results, we demonstrate that the polarity of the solvent is the key factor influencing the Φ(CI) and the photoisomerization yield. © 2011 American Chemical Society

Ultrafast optical ranging using microresonator soliton frequency combs

NASA Astrophysics Data System (ADS)

Trocha, P.; Karpov, M.; Ganin, D.; Pfeiffer, M. H. P.; Kordts, A.; Wolf, S.; Krockenberger, J.; Marin-Palomo, P.; Weimann, C.; Randel, S.; Freude, W.; Kippenberg, T. J.; Koos, C.

2018-02-01

Light detection and ranging is widely used in science and industry. Over the past decade, optical frequency combs were shown to offer advantages in optical ranging, enabling fast distance acquisition with high accuracy. Driven by emerging high-volume applications such as industrial sensing, drone navigation, or autonomous driving, there is now a growing demand for compact ranging systems. Here, we show that soliton Kerr comb generation in integrated silicon nitride microresonators provides a route to high-performance chip-scale ranging systems. We demonstrate dual-comb distance measurements with Allan deviations down to 12 nanometers at averaging times of 13 microseconds along with ultrafast ranging at acquisition rates of 100 megahertz, allowing for in-flight sampling of gun projectiles moving at 150 meters per second. Combining integrated soliton-comb ranging systems with chip-scale nanophotonic phased arrays could enable compact ultrafast ranging systems for emerging mass applications.

Ultrafast Microfluidic Cellular Imaging by Optical Time-Stretch.

PubMed

Lau, Andy K S; Wong, Terence T W; Shum, Ho Cheung; Wong, Kenneth K Y; Tsia, Kevin K

2016-01-01

There is an unmet need in biomedicine for measuring a multitude of parameters of individual cells (i.e., high content) in a large population efficiently (i.e., high throughput). This is particularly driven by the emerging interest in bringing Big-Data analysis into this arena, encompassing pathology, drug discovery, rare cancer cell detection, emulsion microdroplet assays, to name a few. This momentum is particularly evident in recent advancements in flow cytometry. They include scaling of the number of measurable colors from the labeled cells and incorporation of imaging capability to access the morphological information of the cells. However, an unspoken predicament appears in the current technologies: higher content comes at the expense of lower throughput, and vice versa. For example, accessing additional spatial information of individual cells, imaging flow cytometers only achieve an imaging throughput ~1000 cells/s, orders of magnitude slower than the non-imaging flow cytometers. In this chapter, we introduce an entirely new imaging platform, namely optical time-stretch microscopy, for ultrahigh speed and high contrast label-free single-cell (in a ultrafast microfluidic flow up to 10 m/s) imaging and analysis with an ultra-fast imaging line-scan rate as high as tens of MHz. Based on this technique, not only morphological information of the individual cells can be obtained in an ultrafast manner, quantitative evaluation of cellular information (e.g., cell volume, mass, refractive index, stiffness, membrane tension) at nanometer scale based on the optical phase is also possible. The technology can also be integrated with conventional fluorescence measurements widely adopted in the non-imaging flow cytometers. Therefore, these two combinatorial and complementary measurement capabilities in long run is an attractive platform for addressing the pressing need for expanding the "parameter space" in high-throughput single-cell analysis. This chapter provides the

Proton-Based Ultrafast Magic Angle Spinning Solid-State NMR Spectroscopy.

PubMed

Zhang, Rongchun; Mroue, Kamal H; Ramamoorthy, Ayyalusamy

2017-04-18

Protons are vastly abundant in a wide range of exciting macromolecules and thus can be a powerful probe to investigate the structure and dynamics at atomic resolution using solid-state NMR (ssNMR) spectroscopy. Unfortunately, the high signal sensitivity, afforded by the high natural-abundance and high gyromagnetic ratio of protons, is greatly compromised by severe line broadening due to the very strong 1 H- 1 H dipolar couplings. As a result, protons are rarely used, in spite of the desperate need for enhancing the sensitivity of ssNMR to study a variety of systems that are not amenable for high resolution investigation using other techniques including X-ray crystallography, cryo-electron microscopy, and solution NMR spectroscopy. Thanks to the remarkable improvement in proton spectral resolution afforded by the significant advances in magic-angle-spinning (MAS) probe technology, 1 H ssNMR spectroscopy has recently attracted considerable attention in the structural and dynamics studies of various molecular systems. However, it still remains a challenge to obtain narrow 1 H spectral lines, especially from proteins, without resorting to deuteration. In this Account, we review recent proton-based ssNMR strategies that have been developed in our laboratory to further improve proton spectral resolution without resorting to chemical deuteration for the purposes of gaining atomistic-level insights into molecular structures of various crystalline solid systems, using small molecules and peptides as illustrative examples. The proton spectral resolution enhancement afforded by the ultrafast MAS frequencies up to 120 kHz is initially discussed, followed by a description of an ensemble of multidimensional NMR pulse sequences, all based on proton detection, that have been developed to obtain in-depth information from dipolar couplings and chemical shift anisotropy (CSA). Simple single channel multidimensional proton NMR experiments could be performed to probe the proximity of

Ultrafast Non-thermal Response of Plasmonic Resonance in Gold Nanoantennas

NASA Astrophysics Data System (ADS)

Soavi, Giancarlo; Valle, Giuseppe Della; Biagioni, Paolo; Cattoni, Andrea; Longhi, Stefano; Cerullo, Giulio; Brida, Daniele

Ultrafast thermalization of electrons in metal nanostructures is studied by means of pump-probe spectroscopy. We track in real-time the plasmon resonance evolution, providing a tool for understanding and controlling gold nanoantennas non-linear optical response.

Ultrafast electrical spectrum analyzer based on all-optical Fourier transform and temporal magnification.

PubMed

Duan, Yuhua; Chen, Liao; Zhou, Haidong; Zhou, Xi; Zhang, Chi; Zhang, Xinliang

2017-04-03

Real-time electrical spectrum analysis is of great significance for applications involving radio astronomy and electronic warfare, e.g. the dynamic spectrum monitoring of outer space signal, and the instantaneous capture of frequency from other electronic systems. However, conventional electrical spectrum analyzer (ESA) has limited operation speed and observation bandwidth due to the electronic bottleneck. Therefore, a variety of photonics-assisted methods have been extensively explored due to the bandwidth advantage of the optical domain. Alternatively, we proposed and experimentally demonstrated an ultrafast ESA based on all-optical Fourier transform and temporal magnification in this paper. The radio-frequency (RF) signal under test is temporally multiplexed to the spectrum of an ultrashort pulse, thus the frequency information is converted to the time axis. Moreover, since the bandwidth of this ultrashort pulse is far beyond that of the state-of-the-art photo-detector, a temporal magnification system is applied to stretch the time axis, and capture the RF spectrum with 1-GHz resolution. The observation bandwidth of this ultrafast ESA is over 20 GHz, limited by that of the electro-optic modulator. Since all the signal processing is in the optical domain, the acquisition frame rate can be as high as 50 MHz. This ultrafast ESA scheme can be further improved with better dispersive engineering, and is promising for some ultrafast spectral information acquisition applications.

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.

Ultrafast and nonlinear spectroscopy of brilliant green-based nanoGUMBOS with enhanced near-infrared emission

NASA Astrophysics Data System (ADS)

Karam, Tony E.; Siraj, Noureen; Zhang, Zhenyu; Ezzir, Abdulrahman F.; Warner, Isiah M.; Haber, Louis H.

2017-10-01

The synthesis, characterization, ultrafast dynamics, and nonlinear spectroscopy of 30 nm nanospheres of brilliant green-bis(pentafluoroethylsulfonyl)imide ([BG][BETI]) in water are reported. These thermally stable nanoparticles are derived from a group of uniform materials based on organic salts (nanoGUMBOS) that exhibit enhanced near-infrared emission compared with the molecular dye in water. The examination of ultrafast transient absorption spectroscopy results reveals that the overall excited-state relaxation lifetimes of [BG][BETI] nanoGUMBOS are longer than the brilliant green molecular dye in water due to steric hindrance of the torsional degrees of freedom of the phenyl rings around the central carbon. Furthermore, the second harmonic generation signal of [BG][BETI] nanoGUMBOS is enhanced by approximately 7 times and 23 times as compared with colloidal gold nanoparticles of the same size and the brilliant green molecular dye in water, respectively. A very clear third harmonic generation signal is observed from the [BG][BETI] nanoGUMBOS but not from either the molecular dye or the gold nanoparticles. Overall, these results show that [BG][BETI] nanoGUMBOS exhibit altered ultrafast and nonlinear spectroscopy that is beneficial for various applications including nonlinear imaging probes, biomedical imaging, and molecular sensing.

Optically detecting the edge-state of a three-dimensional topological insulator under ambient conditions by ultrafast infrared photoluminescence spectroscopy

PubMed Central

Maezawa, Shun-ya; Watanabe, Hiroshi; Takeda, Masahiro; Kuroda, Kenta; Someya, Takashi; Matsuda, Iwao; Suemoto, Tohru

2015-01-01

Ultrafast infrared photoluminescence spectroscopy was applied to a three-dimensional topological insulator TlBiSe2 under ambient conditions. The dynamics of the luminescence exhibited bulk-insulating and gapless characteristics bounded by the bulk band gap energy. The existence of the topologically protected surface state and the picosecond-order relaxation time of the surface carriers, which was distinguishable from the bulk response, were observed. Our results provide a practical method applicable to topological insulators under ambient conditions for device applications. PMID:26552784

Light, Molecules, Action: Using Ultrafast Uv-Visible and X-Ray Spectroscopy to Probe Excited State Dynamics in Photoactive Molecules

NASA Astrophysics Data System (ADS)

Sension, R. J.

2017-06-01

Light provides a versatile energy source capable of precise manipulation of material systems on size scales ranging from molecular to macroscopic. Photochemistry provides the means for transforming light energy from photon to process via movement of charge, a change in shape, a change in size, or the cleavage of a bond. Photochemistry produces action. In the work to be presented here ultrafast UV-Visible pump-probe, and pump-repump-probe methods have been used to probe the excited state dynamics of stilbene-based molecular motors, cyclohexadiene-based switches, and polyene-based photoacids. Both ultrafast UV-Visible and X-ray absorption spectroscopies have been applied to the study of cobalamin (vitamin B_{12}) based compounds. Optical measurements provide precise characterization of spectroscopic signatures of the intermediate species on the S_{1} surface, while time-resolved XANES spectra at the Co K-edge probe the structural changes that accompany these transformations.

Long-period fiber gratings as ultrafast optical differentiators.

PubMed

Kulishov, Mykola; Azaña, José

2005-10-15

It is demonstrated that a single, uniform long-period fiber grating (LPFG) working in the linear regime inherently behaves as an ultrafast optical temporal differentiator. Specifically, we show that the output temporal waveform in the core mode of a LPFG providing full energy coupling into the cladding mode is proportional to the first derivative of the optical temporal signal (e.g., optical pulse) launched at the input of the LPFG. Moreover, a LPFG providing full energy recoupling back from the cladding mode into the core mode inherently implements second-order temporal differentiation. Our numerical results have confirmed the feasibility of this simple, all-fiber approach to processing optical signals with temporal features in the picosecond and subpicosecond ranges.

Ultrafast optical switching in three-dimensional photonic crystals

NASA Astrophysics Data System (ADS)

Mazurenko, D. A.

2004-09-01

The rapidly expanding research on photonic crystals is driven by potential applications in all-optical switches, optical computers, low-threshold lasers, and holographic data storage. The performance of such devices might surpass the speed of traditional electronics by several orders of magnitude and may result in a true revolution in nanotechnology. The heart of such devices would likely be an optical switching element. This thesis analyzes different regimes of ultrafast all-optical switching in various three-dimensional photonic crystals, in particular opals filled with silicon or vanadium dioxide and periodic arrays of silica-gold core-shell spherical particles with silica outer shell. In the experiment an ultrashort optical pulse is used to excite a photonic crystal and change its complex effective dielectric constant. The change in the imaginary part of the dielectric constant corresponds to the change in absorption that suppresses interference inside the photonic crystal and modifies the amplitude of the reflectivity, while the change in the real part of the dielectric constant accounts for a shift in a spectral position of the photonic stop band. The first type of switching is shown on an example of an opal filled with silicon. In this crystal, switching is induced by photo-excited carriers in silicon that act as an electron plasma and increase the absorption in silicon. Within 30 fs constructive interference inside the opal vanishes and Bragg reflectivity drops down. Changes in reflectivity reach values as high as 46% at maximum excitation power. The experimental results are in a good agreement with calculations. The second type of switching is demonstrated in opal filled with vanadium dioxide. Here, the optical switching is driven by a photoinduced phase transition of vanadium dioxide. The phase transition takes place on a subpicosecond time scale and changes the effective dielectric constant of the opal. As a result, the spectral position of the photonic

Quantum simulation of ultrafast dynamics using trapped ultracold atoms.

PubMed

Senaratne, Ruwan; Rajagopal, Shankari V; Shimasaki, Toshihiko; Dotti, Peter E; Fujiwara, Kurt M; Singh, Kevin; Geiger, Zachary A; Weld, David M

2018-05-25

Ultrafast electronic dynamics are typically studied using pulsed lasers. Here we demonstrate a complementary experimental approach: quantum simulation of ultrafast dynamics using trapped ultracold atoms. Counter-intuitively, this technique emulates some of the fastest processes in atomic physics with some of the slowest, leading to a temporal magnification factor of up to 12 orders of magnitude. In these experiments, time-varying forces on neutral atoms in the ground state of a tunable optical trap emulate the electric fields of a pulsed laser acting on bound charged particles. We demonstrate the correspondence with ultrafast science by a sequence of experiments: nonlinear spectroscopy of a many-body bound state, control of the excitation spectrum by potential shaping, observation of sub-cycle unbinding dynamics during strong few-cycle pulses, and direct measurement of carrier-envelope phase dependence of the response to an ultrafast-equivalent pulse. These results establish cold-atom quantum simulation as a complementary tool for studying ultrafast dynamics.

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

PubMed

Liu, Xiaofeng; Guo, Qiangbing; Qiu, Jianrong

2017-04-01

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

Ultrafast transient grating radiation to optical image converter

DOEpatents

Stewart, Richard E; Vernon, Stephen P; Steel, Paul T; Lowry, Mark E

2014-11-04

A high sensitivity transient grating ultrafast radiation to optical image converter is based on a fixed transmission grating adjacent to a semiconductor substrate. X-rays or optical radiation passing through the fixed transmission grating is thereby modulated and produces a small periodic variation of refractive index or transient grating in the semiconductor through carrier induced refractive index shifts. An optical or infrared probe beam tuned just below the semiconductor band gap is reflected off a high reflectivity mirror on the semiconductor so that it double passes therethrough and interacts with the radiation induced phase grating therein. A small portion of the optical beam is diffracted out of the probe beam by the radiation induced transient grating to become the converted signal that is imaged onto a detector.

Linear and ultrafast nonlinear plasmonics of single nano-objects

NASA Astrophysics Data System (ADS)

Crut, Aurélien; Maioli, Paolo; Vallée, Fabrice; Del Fatti, Natalia

2017-03-01

Single-particle optical investigations have greatly improved our understanding of the fundamental properties of nano-objects, avoiding the spurious inhomogeneous effects that affect ensemble experiments. Correlation with high-resolution imaging techniques providing morphological information (e.g. electron microscopy) allows a quantitative interpretation of the optical measurements by means of analytical models and numerical simulations. In this topical review, we first briefly recall the principles underlying some of the most commonly used single-particle optical techniques: near-field, dark-field, spatial modulation and photothermal microscopies/spectroscopies. We then focus on the quantitative investigation of the surface plasmon resonance (SPR) of metallic nano-objects using linear and ultrafast optical techniques. While measured SPR positions and spectral areas are found in good agreement with predictions based on Maxwell’s equations, SPR widths are strongly influenced by quantum confinement (or, from a classical standpoint, surface-induced electron scattering) and, for small nano-objects, cannot be reproduced using the dielectric functions of bulk materials. Linear measurements on single nano-objects (silver nanospheres and gold nanorods) allow a quantification of the size and geometry dependences of these effects in confined metals. Addressing the ultrafast response of an individual nano-object is also a powerful tool to elucidate the physical mechanisms at the origin of their optical nonlinearities, and their electronic, vibrational and thermal relaxation processes. Experimental investigations of the dynamical response of gold nanorods are shown to be quantitatively modeled in terms of modifications of the metal dielectric function enhanced by plasmonic effects. Ultrafast spectroscopy can also be exploited to unveil hidden physical properties of more complex nanosystems. In this context, two-color femtosecond pump-probe experiments performed on individual

Testing ultrafast mode-locking at microhertz relative optical linewidth.

PubMed

Martin, Michael J; Foreman, Seth M; Schibli, T R; Ye, Jun

2009-01-19

We report new limits on the phase coherence of the ultrafast mode-locking process in an octave-spanning Ti:sapphire comb.We find that the mode-locking mechanism correlates optical phase across a full optical octave with less than 2.5 microHZ relative linewidth. This result is at least two orders of magnitude below recent predictions for quantum-limited individual comb-mode linewidths, verifying that the mode-locking mechanism strongly correlates quantum noise across the comb spectrum.

Ultrafast optical excitations in supramolecular metallacycles with charge transfer properties.

PubMed

Flynn, Daniel C; Ramakrishna, Guda; Yang, Hai-Bo; Northrop, Brian H; Stang, Peter J; Goodson, Theodore

2010-02-03

New organometallic materials such as two-dimensional metallacycles and three-dimensional metallacages are important for the development of novel optical, electronic, and energy related applications. In this article, the ultrafast dynamics of two different platinum-containing metallacycles have been investigated by femtosecond fluorescence upconversion and transient absorption. These measurements were carried out in an effort to probe the charge transfer dynamics and the rate of intersystem crossing in metallacycles of different geometries and dimensions. The processes of ultrafast intersystem crossing and charge transfer vary between the two different classes of metallacyclic systems studied. For rectangular anthracene-containing metallacycles, the electronic coupling between adjacent ligands was relatively weak, whereas for the triangular phenanthrene-containing structures, there was a clear interaction between the conjugated ligand and the metal complex center. The transient lifetimes increased with increasing conjugation in that case. The results show that differences in the dimensionality and structure of metallacycles result in different optical properties, which may be utilized in the design of nonlinear optical materials and potential new, longer-lived excited state materials for further electronic applications.

An Ultrafast Switchable Terahertz Polarization Modulator Based on III-V Semiconductor Nanowires.

PubMed

Baig, Sarwat A; Boland, Jessica L; Damry, Djamshid A; Tan, H Hoe; Jagadish, Chennupati; Joyce, Hannah J; Johnston, Michael B

2017-04-12

Progress in the terahertz (THz) region of the electromagnetic spectrum is undergoing major advances, with advanced THz sources and detectors being developed at a rapid pace. Yet, ultrafast THz communication is still to be realized, owing to the lack of practical and effective THz modulators. Here, we present a novel ultrafast active THz polarization modulator based on GaAs semiconductor nanowires arranged in a wire-grid configuration. We utilize an optical pump-terahertz probe spectroscopy system and vary the polarization of the optical pump beam to demonstrate ultrafast THz modulation with a switching time of less than 5 ps and a modulation depth of -8 dB. We achieve an extinction of over 13% and a dynamic range of -9 dB, comparable to microsecond-switchable graphene- and metamaterial-based THz modulators, and surpassing the performance of optically switchable carbon nanotube THz polarizers. We show a broad bandwidth for THz modulation between 0.1 and 4 THz. Thus, this work presents the first THz modulator which combines not only a large modulation depth but also a broad bandwidth and picosecond time resolution for THz intensity and phase modulation, making it an ideal candidate for ultrafast THz communication.

WS2 mode-locked ultrafast fiber laser

PubMed Central

Mao, Dong; Wang, Yadong; Ma, Chaojie; Han, Lei; Jiang, Biqiang; Gan, Xuetao; Hua, Shijia; Zhang, Wending; Mei, Ting; Zhao, Jianlin

2015-01-01

Graphene-like two dimensional materials, such as WS2 and MoS2, are highly anisotropic layered compounds that have attracted growing interest from basic research to practical applications. Similar with MoS2, few-layer WS2 has remarkable physical properties. Here, we demonstrate for the first time that WS2 nanosheets exhibit ultrafast nonlinear saturable absorption property and high optical damage threshold. Soliton mode-locking operations are achieved separately in an erbium-doped fiber laser using two types of WS2-based saturable absorbers, one of which is fabricated by depositing WS2 nanosheets on a D-shaped fiber, while the other is synthesized by mixing WS2 solution with polyvinyl alcohol, and then evaporating them on a substrate. At the maximum pump power of 600 mW, two saturable absorbers can work stably at mode-locking state without damage, indicating that few-layer WS2 is a promising high-power flexible saturable absorber for ultrafast optics. Numerous applications may benefit from the ultrafast nonlinear features of WS2 nanosheets, such as high-power pulsed laser, materials processing, and frequency comb spectroscopy. PMID:25608729

Ultrafast Charge Transfer in Nickel Phthalocyanine Probed by Femtosecond Raman-Induced Kerr Effect Spectroscopy

PubMed Central

2015-01-01

The recently developed technique of femtosecond stimulated Raman spectroscopy, and its variant, femtosecond Raman-induced Kerr effect spectroscopy (FRIKES), offer access to ultrafast excited-state dynamics via structurally specific vibrational spectra. We have used FRIKES to study the photoexcitation dynamics of nickel(II) phthalocyanine with eight butoxy substituents, NiPc(OBu)8. NiPc(OBu)8 is reported to have a relatively long-lived ligand-to-metal charge-transfer (LMCT) state, an essential characteristic for efficient electron transfer in photocatalysis. Following photoexcitation, vibrational transitions in the FRIKES spectra, assignable to phthalocyanine ring modes, evolve on the femtosecond to picosecond time scales. Correlation of ring core size with the frequency of the ν10 (asymmetric C–N stretching) mode confirms the identity of the LMCT state, which has a ∼500 ps lifetime, as well as that of a precursor d-d excited state. An even earlier (∼0.2 ps) transient is observed and tentatively assigned to a higher-lying Jahn–Teller-active LMCT state. This study illustrates the power of FRIKES spectroscopy in elucidating ultrafast molecular dynamics. PMID:24841906

Broadband atomic-layer MoS₂ optical modulators for ultrafast pulse generations in the visible range.

PubMed

Zhang, Yuxia; Yu, Haohai; Zhang, Rui; Zhao, Gang; Zhang, Huaijin; Chen, Yanxue; Mei, Liangmo; Tonelli, Mauro; Wang, Jiyang

2017-02-01

Visible lasers are a fascinating regime, and their significance is illustrated by the 2014 Noble prizes in physics and chemistry. With the development of blue laser diodes (LDs), the LD-pumped solid-state visible lasers become a burgeoning direction today. Constrained by the scarce visible optical modulators, the solid-state ultrafast visible lasers are rarely realized. Based on the bandgap structure and optoelectronic properties of atomic-layer MoS₂, it can be proposed that MoS₂ has the potential as a visible optical modulator. Here, by originally revealing layer-dependent nonlinear absorption of the atomic-layer MoS₂ in the visible range, broadband atomic-layer MoS₂ optical modulators for the visible ultrafast pulse generation are developed and selected based on the proposed design criteria for novel two-dimensional (2D) optical modulators. By applying the selected MoS₂ optical modulators in the solid-state praseodymium lasers, broadband mode-locked ultrafast lasers from 522 to 639 nm are originally realized. We believe that this Letter should promote the development of visible ultrafast photonics and further applications of 2D optoelectronic materials.

Ultrafast terahertz electrodynamics of photonic and electronic nanostructures

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

Luo, Liang

This thesis summarizes my work on using ultrafast laser pulses to study Terahertz (THz) electrodynamics of photonic and electronic nanostructures and microstructures. Ultrafast timeresolved (optical, NIR, MIR, THz) pump-probe spectroscopy setup has been successfully built, which enables me to perform a series of relevant experiments. Firstly, a novel high e ciency and compact THz wave emitter based on split-ring-resonators has been developed and characterized. The emitter can be pumped at any wavelength by tailoring the magnetic resonance and could generate gapless THz waves covering the entire THz band. Secondly, two kinds of new photonic structures for THz wave manipulation havemore » been successfully designed and characterized. One is based on the 1D and 2D photo-imprinted di ractive elements. The other is based on the photoexcited double-split-ring-resonator metamaterials. Both structures are exible and can modulate THz waves with large tunability. Thirdly, the dark excitons in semiconducting singlewalled carbon nanotubes are studied by optical pump and THz probe spectroscopy, which provides the rst insights into the THz responses of nonequilibrium excitonic correlations and dynamics from the dark ground states in carbon nanotubes. Next, several on-going projects are brie y presented such as the study of ultrafast THz dynamics of Dirac fermions in topological insulator Bi 2Se 3 with Mid-infrared excitation. Finally, the thesis ends with a summary of the completed experiments and an outlook of the future plan.« less

Elucidating ultrafast electron dynamics at surfaces using extreme ultraviolet (XUV) reflection-absorption spectroscopy.

PubMed

Biswas, Somnath; Husek, Jakub; Baker, L Robert

2018-04-24

Here we review the recent development of extreme ultraviolet reflection-absorption (XUV-RA) spectroscopy. This method combines the benefits of X-ray absorption spectroscopy, such as element, oxidation, and spin state specificity, with surface sensitivity and ultrafast time resolution, having a probe depth of only a few nm and an instrument response less than 100 fs. Using this technique we investigated the ultrafast electron dynamics at a hematite (α-Fe2O3) surface. Surface electron trapping and small polaron formation both occur in 660 fs following photoexcitation. These kinetics are independent of surface morphology indicating that electron trapping is not mediated by defects. Instead, small polaron formation is proposed as the likely driving force for surface electron trapping. We also show that in Fe2O3, Co3O4, and NiO, band gap excitation promotes electron transfer from O 2p valence band states to metal 3d conduction band states. In addition to detecting the photoexcited electron at the metal M2,3-edge, the valence band hole is directly observed as transient signal at the O L1-edge. The size of the resulting charge transfer exciton is on the order of a single metal-oxygen bond length. Spectral shifts at the O L1-edge correlate with metal-oxygen bond covalency, confirming the relationship between valence band hybridization and the overpotential for water oxidation. These examples demonstrate the unique ability to measure ultrafast electron dynamics with element and chemical state resolution using XUV-RA spectroscopy. Accordingly, this method is poised to play an important role to reveal chemical details of previously unseen surface electron dynamics.

Nonlinear ultrafast optical response in organic molecular crystals

NASA Astrophysics Data System (ADS)

Rahman, Talat S.; Turkowski, Volodymyr; Leuenberger, Michael N.

2012-02-01

We analyze possible nonlinear excitonic effects in the organic molecule crystals by using a combined time-dependent DFT and many-body approach. In particular, we analyze possible effects of the time-dependent (retarded)interaction between different types of excitations, Frenkel excitons, charge transfer excitons and excimers, on the electric and the optical response of the system. We pay special attention to the case of constant electric field and ultrafast pulses, including that of four-wave mixing experiments. As a specific application we examine the optical excitations of pentacene nanocrystals and compare the results with available experimental data.[1] Our results demostrate that the nonlinear effects can play an important role in the optical response of these systems. [1] A. Kabakchiev, ``Scanning Tunneling Luminescence of Pentacene Nanocrystals'', PhD Thesis (EPFL, Lausanne, 2010).

Ultrafast Airy beam optical parametric oscillator

PubMed Central

Apurv Chaitanya, N.; Kumar, S. Chaitanya; Aadhi, A.; Samanta, G. K.; Ebrahim-Zadeh, M.

2016-01-01

We report on the first realization of an ultrafast Airy beam optical parametric oscillator (OPO). By introducing intracavity cubic phase modulation to the resonant Gaussian signal in a synchronously-pumped singly-resonant OPO cavity and its subsequent Fourier transformation, we have generated 2-dimensional Airy beam in the output signal across a 250 nm tuning range in the near-infrared. The generated Airy beam can be tuned continuously from 1477 to 1727 nm, providing an average power of as much as 306 mW at 1632 nm in pulses of ~23 ps duration with a spectral bandwidth of 1.7 nm. PMID:27476910

Ultrafast electron-optical phonon scattering and quasiparticle lifetime in CVD-grown graphene.

PubMed

Shang, Jingzhi; Yu, Ting; Lin, Jianyi; Gurzadyan, Gagik G

2011-04-26

Ultrafast quasiparticle dynamics in graphene grown by chemical vapor deposition (CVD) has been studied by UV pump/white-light probe spectroscopy. Transient differential transmission spectra of monolayer graphene are observed in the visible probe range (400-650 nm). Kinetics of the quasiparticle (i.e., low-energy single-particle excitation with renormalized energy due to electron-electron Coulomb, electron-optical phonon (e-op), and optical phonon-acoustic phonon (op-ap) interactions) was monitored with 50 fs resolution. Extending the probe range to near-infrared, we find the evolution of quasiparticle relaxation channels from monoexponential e-op scattering to double exponential decay due to e-op and op-ap scattering. Moreover, quasiparticle lifetimes of mono- and randomly stacked graphene films are obtained for the probe photon energies continuously from 1.9 to 2.3 eV. Dependence of quasiparticle decay rate on the probe energy is linear for 10-layer stacked graphene films. This is due to the dominant e-op intervalley scattering and the linear density of states in the probed electronic band. A dimensionless coupling constant W is derived, which characterizes the scattering strength of quasiparticles by lattice points in graphene.

The Dawn of Ultrafast Nonlinear Optics in the Terahertz Regime

NASA Astrophysics Data System (ADS)

Blanchard, F.; Razzari, L.; Su, F. H.; Sharma, G.; Morandotti, Roberto; Ozaki, T.; Reid, M.; Hegmann, F. A.

The terahertz (THz) frequency range is a specific region of the electromagnetic spectrum also known as the far-infrared (FIR) region. More precisely, THz waves cover the region from 100 GHz to 20 THz, thus bridging the gap between microwaves and infrared light. Physically, 1 THz is equivalent to a wavelength of 300 μm in vacuum, to 33.3 cm-1 in terms of wave numbers, to a photon energy of 4 meV, or to a temperature of 48 K. THz waves have the ability to penetrate various materials including non-metallic compounds (papers and plastics), organics, gases, and liquids, thus being a powerful tool for spectroscopic sensing [1]. This portion of the electromagnetic spectrum has been accessible for some time by various means including molecular gas lasers, gyrotrons, and free-electron lasers [2]. Due to complexity, cost, and limited frequencies of operation, these sources have traditionally made it difficult to gain full access to the terahertz frequency range. Nevertheless, there were several pioneering works in nonlinear FIR spectroscopy already in the early 1970s, about one decade after the advent of the laser (readers may find a review in [3]). In particular, saturated absorption in the FIR region was first studied in 1970, which led to the optically pumped FIR gas laser [4]. In the 1980s, the first demonstration of THz radiation coherently generated and detected was made. This result coincided with the development of ultrafast lasers and was obtained using a photoconductive antenna emitter [5], where photoexcited carriers induced by an ultrafast laser pulse are accelerated by a biasing electric field. The resulting time varying current J(t) radiates an electromagnetic transient, E ∝ partial J/partial t , whose amplitude and phase depend on various parameters such as carrier mobility, carrier lifetime, bias field, and on the impurity doping concentration [6]. This allowed the birth of coherent time-domain THz spectroscopy (TDTS) [1], which provided unprecedented

Nonlinear Optical Spectroscopy in the Time Domain: Studies of Ultrafast Molecular Processes in the Condensed Phase.

NASA Astrophysics Data System (ADS)

Joo, Taiha

Ultrafast molecular processes in the condensed phase at room temperature are studied in the time domain by four wave mixing spectroscopy. The structure/dynamics of various quantum states can be studied by varying the time ordering of the incident fields, their polarization, their colors, etc. In one, time-resolved coherent Stokes Raman spectroscopy of benzene is investigated at room temperature. The reorientational correlation time of benzene as well as the T_2 time of the nu _1 ring-breathing mode have been measured by using two different polarization geometries. Bohr frequency difference beats have also been resolved between the nu_1 modes of ^ {12}C_6H_6 and ^{12}C_5^{13 }CH_6.. The dephasing dynamics of the nu _1 ring-breathing mode of neat benzene is studied by time-resolved coherent anti-Stokes Raman scattering. Ultrafast time resolution reveals deviation from the conventional exponential decay. The correlation time, tau _{rm c}, and the rms magnitude, Delta, of the Bohr frequency modulation are determined for the process responsible for the vibrational dephasing by Kubo dephasing function analysis. The electronic dephasing of two oxazine dyes in ethylene glycol at room temperature is investigated by photon echo experiments. It was found that at least two stochastic processes are responsible for the observed electronic dephasing. Both fast (homogeneous) and slow (inhomogeneous) dynamics are recovered using Kubo line shape analysis. Moreover, the slow dynamics is found to spectrally diffuse over the inhomogeneous distribution on the time scale around a picosecond. Time-resolved degenerate four wave mixing signal of dyes in a population measurement geometry is reported. The vibrational coherences both in the ground and excited electronic states produced strong oscillations in the signal together with the usual population decay from the excited electronic state. Absolute frequencies and their dephasing times of the vibrational modes at ~590 cm^{-1} are obtained

Coherent fifth-order visible-infrared spectroscopies: ultrafast nonequilibrium vibrational dynamics in solution.

PubMed

Lynch, Michael S; Slenkamp, Karla M; Cheng, Mark; Khalil, Munira

2012-07-05

Obtaining a detailed description of photochemical reactions in solution requires measuring time-evolving structural dynamics of transient chemical species on ultrafast time scales. Time-resolved vibrational spectroscopies are sensitive probes of molecular structure and dynamics in solution. In this work, we develop doubly resonant fifth-order nonlinear visible-infrared spectroscopies to probe nonequilibrium vibrational dynamics among coupled high-frequency vibrations during an ultrafast charge transfer process using a heterodyne detection scheme. The method enables the simultaneous collection of third- and fifth-order signals, which respectively measure vibrational dynamics occurring on electronic ground and excited states on a femtosecond time scale. Our data collection and analysis strategy allows transient dispersed vibrational echo (t-DVE) and dispersed pump-probe (t-DPP) spectra to be extracted as a function of electronic and vibrational population periods with high signal-to-noise ratio (S/N > 25). We discuss how fifth-order experiments can measure (i) time-dependent anharmonic vibrational couplings, (ii) nonequilibrium frequency-frequency correlation functions, (iii) incoherent and coherent vibrational relaxation and transfer dynamics, and (iv) coherent vibrational and electronic (vibronic) coupling as a function of a photochemical reaction.

Shaping ultrafast laser inscribed optical waveguides using a deformable mirror.

PubMed

Thomson, R R; Bockelt, A S; Ramsay, E; Beecher, S; Greenaway, A H; Kar, A K; Reid, D T

2008-08-18

We use a two-dimensional deformable mirror to shape the spatial profile of an ultrafast laser beam that is then used to inscribe structures in a soda-lime silica glass slide. By doing so we demonstrate that it is possible to control the asymmetry of the cross section of ultrafast laser inscribed optical waveguides via the curvature of the deformable mirror. When tested using 1.55 mum light, the optimum waveguide exhibited coupling losses of approximately 0.2 dB/facet to Corning SMF-28 single mode fiber and propagation losses of approximately 1.5 dB.cm(-1). This technique promises the possibility of combining rapid processing speeds with the ability to vary the waveguide cross section along its length.

Optical nonlinearities and ultrafast all-optical switching of m-plane GaN in the near-infrared

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

Fang, Yu; Zhou, Feng; Yang, Junyi

2015-06-22

We reported a systematic investigation on the three-photon absorption (3PA) spectra and wavelength dispersion of Kerr refraction of bulk m-plane GaN crystal with both polarization E⊥c and E//c by femtosecond Z-scan technique in the near-infrared region from 760 to 1030 nm. Both 3PA spectra and Kerr refraction dispersion were in good agreement with two-band models. The calculated nonlinear figure of merit and measured ultrafast nonlinear refraction dynamics via femtosecond pump-probe with phase object method revealed that m-plane GaN would be a promising candidate for ultrafast all-optical switching and autocorrelation applications at telecommunication wavelengths.

Ultrafast time-resolved spectroscopy of the light-harvesting complex 2 (LH2) from the photosynthetic bacterium Thermochromatium tepidum.

PubMed

Niedzwiedzki, Dariusz M; Fuciman, Marcel; Kobayashi, Masayuki; Frank, Harry A; Blankenship, Robert E

2011-10-01

The light-harvesting complex 2 from the thermophilic purple bacterium Thermochromatium tepidum was purified and studied by steady-state absorption and fluorescence, sub-nanosecond-time-resolved fluorescence and femtosecond time-resolved transient absorption spectroscopy. The measurements were performed at room temperature and at 10 K. The combination of both ultrafast and steady-state optical spectroscopy methods at ambient and cryogenic temperatures allowed the detailed study of carotenoid (Car)-to-bacteriochlorophyll (BChl) as well BChl-to-BChl excitation energy transfer in the complex. The studies show that the dominant Cars rhodopin (N=11) and spirilloxanthin (N=13) do not play a significant role as supportive energy donors for BChl a. This is related with their photophysical properties regulated by long π-electron conjugation. On the other hand, such properties favor some of the Cars, particularly spirilloxanthin (N=13) to play the role of the direct quencher of the excited singlet state of BChl. © Springer Science+Business Media B.V. 2011

Ultra-fast all-optical plasmon induced transparency in a metal–insulator–metal waveguide containing two Kerr nonlinear ring resonators

NASA Astrophysics Data System (ADS)

Nurmohammadi, Tofiq; Abbasian, Karim; Yadipour, Reza

2018-05-01

In this work, an ultra-fast all-optical plasmon induced transparency based on a metal–insulator–metal nanoplasmonic waveguide with two Kerr nonlinear ring resonators is studied. Two-dimensional simulations utilizing the finite-difference time-domain method are used to show an obvious optical bistability and significant switching mechanisms of the signal light by varying the pump-light intensity. The proposed all-optical switching based on plasmon induced transparency demonstrates femtosecond-scale feedback time (90 fs), meaning ultra-fast switching can be achieved. The presented all-optical switch may have potential significant applications in integrated optical circuits.

Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy.

PubMed

Hayes, Dugan; Kohler, Lars; Hadt, Ryan G; Zhang, Xiaoyi; Liu, Cunming; Mulfort, Karen L; Chen, Lin X

2018-01-28

The kinetics of photoinduced electron and energy transfer in a family of tetrapyridophenazine-bridged heteroleptic homo- and heterodinuclear copper(i) bis(phenanthroline)/ruthenium(ii) polypyridyl complexes were studied using ultrafast optical and multi-edge X-ray transient absorption spectroscopies. This work combines the synthesis of heterodinuclear Cu(i)-Ru(ii) analogs of the homodinuclear Cu(i)-Cu(i) targets with spectroscopic analysis and electronic structure calculations to first disentangle the dynamics at individual metal sites by taking advantage of the element and site specificity of X-ray absorption and theoretical methods. The excited state dynamical models developed for the heterodinuclear complexes are then applied to model the more challenging homodinuclear complexes. These results suggest that both intermetallic charge and energy transfer can be observed in an asymmetric dinuclear copper complex in which the ground state redox potentials of the copper sites are offset by only 310 meV. We also demonstrate the ability of several of these complexes to effectively and unidirectionally shuttle energy between different metal centers, a property that could be of great use in the design of broadly absorbing and multifunctional multimetallic photocatalysts. This work provides an important step toward developing both a fundamental conceptual picture and a practical experimental handle with which synthetic chemists, spectroscopists, and theoreticians may collaborate to engineer cheap and efficient photocatalytic materials capable of performing coulombically demanding chemical transformations.

Capturing Structural Snapshots during Photochemical Reactions with Ultrafast Raman Spectroscopy: From Materials Transformation to Biosensor Responses.

PubMed

Fang, Chong; Tang, Longteng; Oscar, Breland G; Chen, Cheng

2018-06-21

Chemistry studies the composition, structure, properties, and transformation of matter. A mechanistic understanding of the pertinent processes is required to translate fundamental knowledge into practical applications. The current development of ultrafast Raman as a powerful time-resolved vibrational technique, particularly femtosecond stimulated Raman spectroscopy (FSRS), has shed light on the structure-energy-function relationships of various photosensitive systems. This Perspective reviews recent work incorporating optical innovations, including the broad-band up-converted multicolor array (BUMA) into a tunable FSRS setup, and demonstrates its resolving power to watch metal speciation and photolysis, leading to high-quality thin films, and fluorescence modulation of chimeric protein biosensors for calcium ion imaging. We discuss advantages of performing FSRS in the mixed time-frequency domain and present strategies to delineate mechanisms by tracking low-frequency modes and systematically modifying chemical structures with specific functional groups. These unique insights at the chemical-bond level have started to enable the rational design and precise control of functional molecular machines in optical, materials, energy, and life sciences.

Characterization of Ultrafast Laser Pulses using a Low-dispersion Frequency Resolved Optical Grating Spectrometer

NASA Astrophysics Data System (ADS)

Whitelock, Hope; Bishop, Michael; Khosravi, Soroush; Obaid, Razib; Berrah, Nora

2016-05-01

A low dispersion frequency-resolved optical gating (FROG) spectrometer was designed to characterize ultrashort (<50 femtosecond) laser pulses from a commercial regenerative amplifier, optical parametric amplifier, and a home-built non-colinear optical parametric amplifier. This instrument splits a laser pulse into two replicas with a 90:10 intensity ratio using a thin pellicle beam-splitter and then recombines the pulses in a birefringent medium. The instrument detects a wavelength-sensitive change in polarization of the weak probe pulse in the presence of the stronger pump pulse inside the birefringent medium. Scanning the time delay between the two pulses and acquiring spectra allows for characterization of the frequency and time content of ultrafast laser pulses, that is needed for interpretation of experimental results obtained from these ultrafast laser systems. Funded by the DoE-BES, Grant No. DE-SC0012376.

Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

DOE PAGES

Rouxel, Jérémy R.; Kowalewski, Markus; Mukamel, Shaul

2017-07-01

Recently developed circularly polarized X-ray light sources can probe the ultrafast chiral electronic and nuclear dynamics through spatially localized resonant core transitions. Here, we present simulations of time-resolved circular dichroism signals given by the difference of left and right circularly polarized X-ray probe transmission following an excitation by a circularly polarized optical pump with the variable time delay. Application is made to formamide which is achiral in the ground state and assumes two chiral geometries upon optical excitation to the first valence excited state. Probes resonant with various K-edges (C, N, and O) provide different local windows onto the paritymore » breaking geometry change thus revealing the enantiomer asymmetry.« less

Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

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

Rouxel, Jérémy R.; Kowalewski, Markus; Mukamel, Shaul

Recently developed circularly polarized X-ray light sources can probe the ultrafast chiral electronic and nuclear dynamics through spatially localized resonant core transitions. Here, we present simulations of time-resolved circular dichroism signals given by the difference of left and right circularly polarized X-ray probe transmission following an excitation by a circularly polarized optical pump with the variable time delay. Application is made to formamide which is achiral in the ground state and assumes two chiral geometries upon optical excitation to the first valence excited state. Probes resonant with various K-edges (C, N, and O) provide different local windows onto the paritymore » breaking geometry change thus revealing the enantiomer asymmetry.« less

Ultrafast core-loss spectroscopy in four-dimensional electron microscopy

PubMed Central

van der Veen, Renske M.; Penfold, Thomas J.; Zewail, Ahmed H.

2015-01-01

We demonstrate ultrafast core-electron energy-loss spectroscopy in four-dimensional electron microscopy as an element-specific probe of nanoscale dynamics. We apply it to the study of photoexcited graphite with femtosecond and nanosecond resolutions. The transient core-loss spectra, in combination with ab initio molecular dynamics simulations, reveal the elongation of the carbon-carbon bonds, even though the overall behavior is a contraction of the crystal lattice. A prompt energy-gap shrinkage is observed on the picosecond time scale, which is caused by local bond length elongation and the direct renormalization of band energies due to temperature-dependent electron–phonon interactions. PMID:26798793

Ultrafast Spectral Photoresponse of Bilayer Graphene: Optical Pump-Terahertz Probe Spectroscopy.

PubMed

Kar, Srabani; Nguyen, Van Luan; Mohapatra, Dipti R; Lee, Young Hee; Sood, A K

2018-02-27

Photoinduced terahertz conductivity Δσ(ω) of Bernal stacked bilayer graphene (BLG) with different dopings is measured by time-resolved optical pump terahertz probe spectroscopy. The real part of photoconductivity Δσ(ω) (Δσ Re (ω)) is positive throughout the spectral range 0.5-2.5 THz in low-doped BLG. This is in sharp contrast to Δσ(ω) for high-doped bilayer graphene where Δσ Re (ω) is negative at low frequency and positive on the high frequency side. We use Boltzmann transport theory to understand quantitatively the frequency dependence of Δσ(ω), demanding the energy dependence of different scattering rates such as short-range impurity scattering, Coulomb scattering, carrier-acoustic phonon scattering, and substrate surface optical phonon scattering. We find that the short-range disorder scattering dominates over other processes. The calculated photoconductivity captures very well the experimental conductivity spectra as a function of lattice temperature varying from 300 to 4 K, without any empirical fitting procedures adopted so far in the literature. This helps us to understand the intraband conductivity of photoexcited hot carriers in 2D materials.

Ultrafast Nanoimaging of the Photoinduced Phase Transition Dynamics in VO2.

PubMed

Dönges, Sven A; Khatib, Omar; O'Callahan, Brian T; Atkin, Joanna M; Park, Jae Hyung; Cobden, David; Raschke, Markus B

2016-05-11

Many phase transitions in correlated matter exhibit spatial inhomogeneities with expected yet unexplored effects on the associated ultrafast dynamics. Here we demonstrate the combination of ultrafast nondegenerate pump-probe spectroscopy with far from equilibrium excitation, and scattering scanning near-field optical microscopy (s-SNOM) for ultrafast nanoimaging. In a femtosecond near-field near-IR (NIR) pump and mid-IR (MIR) probe study, we investigate the photoinduced insulator-to-metal (IMT) transition in nominally homogeneous VO2 microcrystals. With pump fluences as high as 5 mJ/cm(2), we can reach three distinct excitation regimes. We observe a spatial heterogeneity on ∼50-100 nm length scales in the fluence-dependent IMT dynamics ranging from <100 fs to ∼1 ps. These results suggest a high sensitivity of the IMT with respect to small local variations in strain, doping, or defects that are difficult to discern microscopically. We provide a perspective with the distinct requirements and considerations of ultrafast spatiotemporal nanoimaging of phase transitions in quantum materials.

High Harmonic Generation XUV Spectroscopy for Studying Ultrafast Photophysics of Coordination Complexes

NASA Astrophysics Data System (ADS)

Ryland, Elizabeth S.; Lin, Ming-Fu; Benke, Kristin; Verkamp, Max A.; Zhang, Kaili; Vura-Weis, Josh

2017-06-01

Extreme ultraviolet (XUV) spectroscopy is an inner shell technique that probes the M_{2,3}-edge excitation of atoms. Absorption of the XUV photon causes a 3p→3d transition, the energy and shape of which is directly related to the element and ligand environment. This technique is thus element-, oxidation state-, spin state-, and ligand field specific. A process called high-harmonic generation (HHG) enables the production of ultrashort (˜20fs) pulses of collimated XUV photons in a tabletop instrument. This allows transient XUV spectroscopy to be conducted as an in-lab experiment, where it was previously only possible at accelerator-based light sources. Additionally, ultrashort pulses provide the capability for unprecedented time resolution (˜50fs IRF). This technique has the capacity to serve a pivotal role in the study of electron and energy transfer processes in materials and chemical biology. I will present the XUV transient absorption instrument we have built, along with ultrafast transient M_{2,3}-edge absorption data of a series of small inorganic molecules in order to demonstrate the high specificity and time resolution of this tabletop technique as well as how our group is applying it to the study of ultrafast electronic dynamics of coordination complexes.

Clean sub-8-fs pulses at 400 nm generated by a hollow fiber compressor for ultraviolet ultrafast pump-probe spectroscopy.

PubMed

Liu, Jun; Okamura, Kotaro; Kida, Yuichiro; Teramoto, Takahiro; Kobayashi, Takayoshi

2010-09-27

Clean 7.5 fs pulses at 400 nm with less than 3% energy in tiny satellite pulses were obtained by spectral broadening in a hollow fiber and dispersive compensating using a prism pair together with a deformable mirror system. As an example, this stable and clean pulse was used to study the ultrafast pump-probe spectroscopy of photoactive yellow protein. Moreover, the self-diffraction signal shows a smoothed and broadened laser spectrum and is expected to have a further clean laser pulse, which makes it more useful in the ultrafast pump-probe spectroscopy in the future.

Noncollinear generation of optical spatiotemporal solitons and application to ultrafast digital logic

NASA Astrophysics Data System (ADS)

Liu, Xiang; Beckwitt, Kale; Wise, Frank

2000-05-01

We demonstrate theoretically and experimentally that spatiotemporal solitons can be generated through noncollinear second-harmonic generation. The resulting Y geometry could be used to implement an optical AND gate with ultrafast, high-contrast operation but without sensitivity to the phases of the input pulses.

Ultrafast Multi-Level Logic Gates with Spin-Valley Coupled Polarization Anisotropy in Monolayer MoS2

PubMed Central

Wang, Yu-Ting; Luo, Chih-Wei; Yabushita, Atsushi; Wu, Kaung-Hsiung; Kobayashi, Takayoshi; Chen, Chang-Hsiao; Li, Lain-Jong

2015-01-01

The inherent valley-contrasting optical selection rules for interband transitions at the K and K′ valleys in monolayer MoS2 have attracted extensive interest. Carriers in these two valleys can be selectively excited by circularly polarized optical fields. The comprehensive dynamics of spin valley coupled polarization and polarized exciton are completely resolved in this work. Here, we present a systematic study of the ultrafast dynamics of monolayer MoS2 including spin randomization, exciton dissociation, free carrier relaxation, and electron-hole recombination by helicity- and photon energy-resolved transient spectroscopy. The time constants for these processes are 60 fs, 1 ps, 25 ps, and ~300 ps, respectively. The ultrafast dynamics of spin polarization, valley population, and exciton dissociation provides the desired information about the mechanism of radiationless transitions in various applications of 2D transition metal dichalcogenides. For example, spin valley coupled polarization provides a promising way to build optically selective-driven ultrafast valleytronics at room temperature. Therefore, a full understanding of the ultrafast dynamics in MoS2 is expected to provide important fundamental and technological perspectives. PMID:25656222

Coherent Amplification of Ultrafast Molecular Dynamics in an Optical Oscillator

NASA Astrophysics Data System (ADS)

Aharonovich, Igal; Pe'er, Avi

2016-02-01

Optical oscillators present a powerful optimization mechanism. The inherent competition for the gain resources between possible modes of oscillation entails the prevalence of the most efficient single mode. We harness this "ultrafast" coherent feedback to optimize an optical field in time, and show that, when an optical oscillator based on a molecular gain medium is synchronously pumped by ultrashort pulses, a temporally coherent multimode field can develop that optimally dumps a general, dynamically evolving vibrational wave packet, into a single vibrational target state. Measuring the emitted field opens a new window to visualization and control of fast molecular dynamics. The realization of such a coherent oscillator with hot alkali dimers appears within experimental reach.

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium.

PubMed

Zürch, Michael; Chang, Hung-Tzu; Borja, Lauren J; Kraus, Peter M; Cushing, Scott K; Gandman, Andrey; Kaplan, Christopher J; Oh, Myoung Hwan; Prell, James S; Prendergast, David; Pemmaraju, Chaitanya D; Neumark, Daniel M; Leone, Stephen R

2017-06-01

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M 4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 10 20  cm -3 . Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first-order electron and hole decay of ∼1 ps suggests a Shockley-Read-Hall recombination mechanism. The simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium

PubMed Central

Zürch, Michael; Chang, Hung-Tzu; Borja, Lauren J.; Kraus, Peter M.; Cushing, Scott K.; Gandman, Andrey; Kaplan, Christopher J.; Oh, Myoung Hwan; Prell, James S.; Prendergast, David; Pemmaraju, Chaitanya D.; Neumark, Daniel M.; Leone, Stephen R.

2017-01-01

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 1020 cm−3. Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first-order electron and hole decay of ∼1 ps suggests a Shockley–Read–Hall recombination mechanism. The simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions. PMID:28569752

Ultrafast-based projection-reconstruction three-dimensional nuclear magnetic resonance spectroscopy.

PubMed

Mishkovsky, Mor; Kupce, Eriks; Frydman, Lucio

2007-07-21

Recent years have witnessed increased efforts toward the accelerated acquisition of multidimensional nuclear magnetic resonance (nD NMR) spectra. Among the methods proposed to speed up these NMR experiments is "projection reconstruction," a scheme based on the acquisition of a reduced number of two-dimensional (2D) NMR data sets constituting cross sections of the nD time domain being sought. Another proposition involves "ultrafast" spectroscopy, capable of completing nD NMR acquisitions within a single scan. Potential limitations of these approaches include the need for a relatively slow 2D-type serial data collection procedure in the former case, and a need for at least n high-performance, linearly independent gradients and a sufficiently high sensitivity in the latter. The present study introduces a new scheme that comes to address these limitations, by combining the basic features of the projection reconstruction and the ultrafast approaches into a single, unified nD NMR experiment. In the resulting method each member within the series of 2D cross sections required by projection reconstruction to deliver the nD NMR spectrum being sought, is acquired within a single scan with the aid of the 2D ultrafast protocol. Full nD NMR spectra can thus become available by backprojecting a small number of 2D sets, collected using a minimum number of scans. Principles, opportunities, and limitations of the resulting approach, together with demonstrations of its practical advantages, are here discussed and illustrated with a series of three-dimensional homo- and heteronuclear NMR correlation experiments.

Modeling of coherent ultrafast magneto-optical experiments: Light-induced molecular mean-field model

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

Hinschberger, Y.; Hervieux, P.-A.

2015-12-28

We present calculations which aim to describe coherent ultrafast magneto-optical effects observed in time-resolved pump-probe experiments. Our approach is based on a nonlinear semi-classical Drude-Voigt model and is used to interpret experiments performed on nickel ferromagnetic thin film. Within this framework, a phenomenological light-induced coherent molecular mean-field depending on the polarizations of the pump and probe pulses is proposed whose microscopic origin is related to a spin-orbit coupling involving the electron spins of the material sample and the electric field of the laser pulses. Theoretical predictions are compared to available experimental data. The model successfully reproduces the observed experimental trendsmore » and gives meaningful insight into the understanding of magneto-optical rotation behavior in the ultrafast regime. Theoretical predictions for further experimental studies are also proposed.« less

Ultrafast Terahertz Nonlinear Optics of Landau Level Transitions in a Monolayer Graphene

NASA Astrophysics Data System (ADS)

Yumoto, Go; Matsunaga, Ryusuke; Hibino, Hiroki; Shimano, Ryo

2018-03-01

We investigated the ultrafast terahertz (THz) nonlinearity in a monolayer graphene under the strong magnetic field using THz pump-THz probe spectroscopy. An ultrafast suppression of the Faraday rotation associated with inter-Landau level (LL) transitions is observed, reflecting the Dirac electron character of nonequidistant LLs with large transition dipole moments. A drastic modulation of electron distribution in LLs is induced by far off-resonant THz pulse excitation in the transparent region. Numerical simulation based on the density matrix formalism without rotating-wave approximation reproduces the experimental results. Our results indicate that the strong light-matter coupling regime is realized in graphene, with the Rabi frequency exceeding the carrier wave frequency and even the relevant energy scale of the inter-LL transition.

Unraveling shock-induced chemistry using ultrafast lasers

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

Moore, David Steven

The exquisite time synchronicity between shock and diagnostics needed to unravel chemical events occurring in picoseconds has been achieved using a shaped ultrafast laser pulse to both drive the shocks and interrogate the sample via a multiplicity of optical diagnostics. The shaped laser drive pulse can produce well-controlled shock states of sub-ns duration with sub-10 ps risetimes, sufficient for investigation offast reactions or phase transformations in a thin layer with picosecond time resolution. The shock state is characterized using ultrafast dynamic ellipsometry (UDE) in either planar or Gaussian spatial geometries, the latter allowing measurements of the equation of state ofmore » materials at a range of stresses in a single laser pulse. Time-resolved processes in materials are being interrogated using UDE, ultrafast infrared absorption, ultrafast UV/visible absorption, and femtosecond stimulated Raman spectroscopy. Using these tools we showed that chemistry in an energetic thin film starts only after an induction time of a few tens of ps, an observation that allows differentiation between proposed shock-induced reaction mechanisms. These tools are presently being applied to a variety of energetic and reactive sample systems, from nitromethane and carbon disulfide, to microengineered interfaces in tunable energetic mixtures. Recent results will be presented, and future trends outlined.« less

Electro-optic deflectors deliver advantages over acousto-optical deflectors in a high resolution, ultra-fast force-clamp optical trap.

PubMed

Woody, Michael S; Capitanio, Marco; Ostap, E Michael; Goldman, Yale E

2018-04-30

We characterized experimental artifacts arising from the non-linear response of acousto-optical deflectors (AODs) in an ultra-fast force-clamp optical trap and have shown that using electro-optical deflectors (EODs) instead eliminates these artifacts. We give an example of the effects of these artifacts in our ultra-fast force clamp studies of the interaction of myosin with actin filaments. The experimental setup, based on the concept of Capitanio et al. [Nat. Methods 9, 1013-1019 (2012)] utilizes a bead-actin-bead dumbbell held in two force-clamped optical traps which apply a load to the dumbbell to move it at a constant velocity. When myosin binds to actin, the filament motion stops quickly as the total force from the optical traps is transferred to the actomyosin attachment. We found that in our setup, AODs were unsuitable for beam steering due to non-linear variations in beam intensity and deflection angle as a function of driving frequency, likely caused by low-amplitude standing acoustic waves in the deflectors. These aberrations caused instability in the force feedback loops leading to artifactual jumps in the trap position. We demonstrate that beam steering with EODs improves the performance of our instrument. Combining the superior beam-steering capability of the EODs, force acquisition via back-focal-plane interferometry, and dual high-speed FPGA-based feedback loops, we apply precise and constant loads to study the dynamics of interactions between actin and myosin. The same concept applies to studies of other biomolecular interactions.

Characterization of photo-induced valence tautomerism in a cobalt-dioxolene complex by ultrafast spectroscopy

NASA Astrophysics Data System (ADS)

Beni, A.; Bogani, L.; Bussotti, L.; Dei, A.; Gentili, P. L.; Righini, R.

2005-01-01

The valence tautomerism of low-spin CoIII(Cat-N-BQ)(Cat-N-SQ) was investigated by means of UV-vis pump-probe transient absorption spectroscopy in chloroform. By exciting the CT transition of the complex at 480 nm, an intramolecular electron transfer process is selectively triggered. The photo-induced charge transfer is pursued by a cascade of two main molecular events characterized by the ultrafast transient absorption spectroscopy: the first gives rise to the metastable high-spin CoII(Cat-N-BQ)2 that, secondly, reaches the chemical equilibrium with the reactant species.

Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy

DOE PAGES

Hayes, Dugan; Kohler, Lars; Hadt, Ryan G.; ...

2017-11-28

Here, the kinetics of photoinduced electron and energy transfer in a family of tetrapyridophenazine-bridged heteroleptic homo- and heterodinuclear copper(I) bis(phenanthroline)/ruthenium(II) polypyridyl complexes were studied using ultrafast optical and multi-edge X-ray transient absorption spectroscopies. This work combines the synthesis of heterodinuclear Cu(I)–Ru(II) analogs of the homodinuclear Cu(I)–Cu(I) targets with spectroscopic analysis and electronic structure calculations to first disentangle the dynamics at individual metal sites by taking advantage of the element and site specificity of X-ray absorption and theoretical methods. The excited state dynamical models developed for the heterodinuclear complexes are then applied to model the more challenging homodinuclear complexes. These resultsmore » suggest that both intermetallic charge and energy transfer can be observed in an asymmetric dinuclear copper complex in which the ground state redox potentials of the copper sites are offset by only 310 meV. We also demonstrate the ability of several of these complexes to effectively and unidirectionally shuttle energy between different metal centers, a property that could be of great use in the design of broadly absorbing and multifunctional multimetallic photocatalysts. This work provides an important step toward developing both a fundamental conceptual picture and a practical experimental handle with which synthetic chemists, spectroscopists, and theoreticians may collaborate to engineer cheap and efficient photocatalytic materials capable of performing coulombically demanding chemical transformations.« less

Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy

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

Hayes, Dugan; Kohler, Lars; Hadt, Ryan G.

Here, the kinetics of photoinduced electron and energy transfer in a family of tetrapyridophenazine-bridged heteroleptic homo- and heterodinuclear copper(I) bis(phenanthroline)/ruthenium(II) polypyridyl complexes were studied using ultrafast optical and multi-edge X-ray transient absorption spectroscopies. This work combines the synthesis of heterodinuclear Cu(I)–Ru(II) analogs of the homodinuclear Cu(I)–Cu(I) targets with spectroscopic analysis and electronic structure calculations to first disentangle the dynamics at individual metal sites by taking advantage of the element and site specificity of X-ray absorption and theoretical methods. The excited state dynamical models developed for the heterodinuclear complexes are then applied to model the more challenging homodinuclear complexes. These resultsmore » suggest that both intermetallic charge and energy transfer can be observed in an asymmetric dinuclear copper complex in which the ground state redox potentials of the copper sites are offset by only 310 meV. We also demonstrate the ability of several of these complexes to effectively and unidirectionally shuttle energy between different metal centers, a property that could be of great use in the design of broadly absorbing and multifunctional multimetallic photocatalysts. This work provides an important step toward developing both a fundamental conceptual picture and a practical experimental handle with which synthetic chemists, spectroscopists, and theoreticians may collaborate to engineer cheap and efficient photocatalytic materials capable of performing coulombically demanding chemical transformations.« less

Ultrafast frequency-agile terahertz devices using methylammonium lead halide perovskites.

PubMed

Chanana, Ashish; Liu, Xiaojie; Zhang, Chuang; Vardeny, Zeev Valy; Nahata, Ajay

2018-05-01

The ability to control the response of metamaterial structures can facilitate the development of new terahertz devices, with applications in spectroscopy and communications. We demonstrate ultrafast frequency-agile terahertz metamaterial devices that enable such a capability, in which multiple perovskites can be patterned in each unit cell with micrometer-scale precision. To accomplish this, we developed a fabrication technique that shields already deposited perovskites from organic solvents, allowing for multiple perovskites to be patterned in close proximity. By doing so, we demonstrate tuning of the terahertz resonant response that is based not only on the optical pump fluence but also on the optical wavelength. Because polycrystalline perovskites have subnanosecond photocarrier recombination lifetimes, switching between resonances can occur on an ultrafast time scale. The use of multiple perovskites allows for new functionalities that are not possible using a single semiconducting material. For example, by patterning one perovskite in the gaps of split-ring resonators and bringing a uniform thin film of a second perovskite in close proximity, we demonstrate tuning of the resonant response using one optical wavelength and suppression of the resonance using a different optical wavelength. This general approach offers new capabilities for creating tunable terahertz devices.

QoS support over ultrafast TDM optical networks

NASA Astrophysics Data System (ADS)

Narvaez, Paolo; Siu, Kai-Yeung; Finn, Steven G.

1999-08-01

HLAN is a promising architecture to realize Tb/s access networks based on ultra-fast optical TDM technologies. This paper presents new research results on efficient algorithms for the support of quality of service over the HLAN network architecture. In particular, we propose a new scheduling algorithm that emulates fair queuing in a distributed manner for bandwidth allocation purpose. The proposed scheduler collects information on the queue of each host on the network and then instructs each host how much data to send. Our new scheduling algorithm ensures full bandwidth utilization, while guaranteeing fairness among all hosts.

Theoretical ultra-fast spectroscopy in transition metal dichalcogenides

NASA Astrophysics Data System (ADS)

Molina-Sanchez, Alejandro; Sangalli, Davide; Marini, Andrea; Wirtz, Ludger

Semiconducting 2D-materials like the transition metal dichalcogenides (TMDs) MoS2, MoSe2, WS2, WSe2 are promising alternatives to graphene for designing novel opto-electronic devices. The strong spin-orbit interaction along with the breaking of inversion symmetry in single-layer TMDs allow using the valley-index as a new quantum number. The practical use of valley physics depends on the lifetimes of valley-polarized excitons which are affected by scattering at phonons, impurities and by carrier-carrier interactions. The carrier dynamics can be monitored using ultra-fast spectroscopies such as pump-probe experiments. The carrier dynamics is simulated using non-equilibrium Green's function theory in an ab-initio framework. We include carrier relaxation through electron-phonon interaction. We obtain the transient absorption spectra of single-layer TMD and compare our simulations with recent pump-probe experiments

Ultrafast relaxation dynamics of nitric oxide synthase studied by visible broadband transient absorption spectroscopy

NASA Astrophysics Data System (ADS)

Hung, Chih-Chang; Yabushita, Atsushi; Kobayashi, Takayoshi; Chen, Pei-Feng; Liang, Keng S.

2017-09-01

Ultrafast dynamics of endothelial nitric oxide synthase (eNOS) oxygenase domain was studied by transient absorption spectroscopy pumping at Soret band. The broadband visible probe spectrum has visualized the relaxation dynamics from the Soret band to Q-band and charge transfer (CT) band. Supported by two-dimensional correlation spectroscopy, global fitting analysis has successfully concluded the relaxation dynamics from the Soret band to be (1) electronic transition to Q-band (0.16 ps), (2) ligand dissociation and CT (0.94 ps), (3) relaxation of the CT state (4.0 ps), and (4) ligand rebinding (59 ps).

Laser plasma x-ray source for ultrafast time-resolved x-ray absorption spectroscopy

DOE PAGES

Miaja-Avila, L.; O'Neil, G. C.; Uhlig, J.; ...

2015-03-02

We describe a laser-driven x-ray plasma source designed for ultrafast x-ray absorption spectroscopy. The source is comprised of a 1 kHz, 20 W, femtosecond pulsed infrared laser and a water target. We present the x-ray spectra as a function of laser energy and pulse duration. Additionally, we investigate the plasma temperature and photon flux as we vary the laser energy. We obtain a 75 μm FWHM x-ray spot size, containing ~10 6 photons/s, by focusing the produced x-rays with a polycapillary optic. Since the acquisition of x-ray absorption spectra requires the averaging of measurements from >10 7 laser pulses, wemore » also present data on the source stability, including single pulse measurements of the x-ray yield and the x-ray spectral shape. In single pulse measurements, the x-ray flux has a measured standard deviation of 8%, where the laser pointing is the main cause of variability. Further, we show that the variability in x-ray spectral shape from single pulses is low, thus justifying the combining of x-rays obtained from different laser pulses into a single spectrum. Finally, we show a static x-ray absorption spectrum of a ferrioxalate solution as detected by a microcalorimeter array. Altogether, our results demonstrate that this water-jet based plasma source is a suitable candidate for laboratory-based time-resolved x-ray absorption spectroscopy experiments.« less

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

PubMed

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

2009-07-01

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

Ultrafast wavelength multiplexed broad bandwidth digital diffuse optical spectroscopy for in vivo extraction of tissue optical properties

NASA Astrophysics Data System (ADS)

Torjesen, Alyssa; Istfan, Raeef; Roblyer, Darren

2017-03-01

Frequency-domain diffuse optical spectroscopy (FD-DOS) utilizes intensity-modulated light to characterize optical scattering and absorption in thick tissue. Previous FD-DOS systems have been limited by large device footprints, complex electronics, high costs, and limited acquisition speeds, all of which complicate access to patients in the clinical setting. We have developed a new digital DOS (dDOS) system, which is relatively compact and inexpensive, allowing for simplified clinical use, while providing unprecedented measurement speeds. The dDOS system utilizes hardware-integrated custom board-level direct digital synthesizers and an analog-to-digital converter to generate frequency sweeps and directly measure signals utilizing undersampling at six wavelengths modulated at discrete frequencies from 50 to 400 MHz. Wavelength multiplexing is utilized to achieve broadband frequency sweep measurements acquired at over 97 Hz. When compared to a gold-standard DOS system, the accuracy of optical properties recovered with the dDOS system was within 5.3% and 5.5% for absorption and reduced scattering coefficient extractions, respectively. When tested in vivo, the dDOS system was able to detect physiological changes throughout the cardiac cycle. The new FD-dDOS system is fast, inexpensive, and compact without compromising measurement quality.

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium

DOE PAGES

Zurch, Michael; Chang, Hung -Tzu; Borja, Lauren J.; ...

2017-06-01

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M 4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 10 20 cm –3. Separate electron and hole relaxation times are observedmore » as a function of hot carrier energies. A first-order electron and hole decay of ~1 ps suggests a Shockley–Read–Hall recombination mechanism. Furthermore, the simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.« less

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium

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

Zurch, Michael; Chang, Hung -Tzu; Borja, Lauren J.

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M 4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 10 20 cm –3. Separate electron and hole relaxation times are observedmore » as a function of hot carrier energies. A first-order electron and hole decay of ~1 ps suggests a Shockley–Read–Hall recombination mechanism. Furthermore, the simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.« less

Ultrafast Graphene Light Emitters.

PubMed

Kim, Young Duck; Gao, Yuanda; Shiue, Ren-Jye; Wang, Lei; Aslan, Ozgur Burak; Bae, Myung-Ho; Kim, Hyungsik; Seo, Dongjea; Choi, Heon-Jin; Kim, Suk Hyun; Nemilentsau, Andrei; Low, Tony; Tan, Cheng; Efetov, Dmitri K; Taniguchi, Takashi; Watanabe, Kenji; Shepard, Kenneth L; Heinz, Tony F; Englund, Dirk; Hone, James

2018-02-14

Ultrafast electrically driven nanoscale light sources are critical components in nanophotonics. Compound semiconductor-based light sources for the nanophotonic platforms have been extensively investigated over the past decades. However, monolithic ultrafast light sources with a small footprint remain a challenge. Here, we demonstrate electrically driven ultrafast graphene light emitters that achieve light pulse generation with up to 10 GHz bandwidth across a broad spectral range from the visible to the near-infrared. The fast response results from ultrafast charge-carrier dynamics in graphene and weak electron-acoustic phonon-mediated coupling between the electronic and lattice degrees of freedom. We also find that encapsulating graphene with hexagonal boron nitride (hBN) layers strongly modifies the emission spectrum by changing the local optical density of states, thus providing up to 460% enhancement compared to the gray-body thermal radiation for a broad peak centered at 720 nm. Furthermore, the hBN encapsulation layers permit stable and bright visible thermal radiation with electronic temperatures up to 2000 K under ambient conditions as well as efficient ultrafast electronic cooling via near-field coupling to hybrid polaritonic modes under electrical excitation. These high-speed graphene light emitters provide a promising path for on-chip light sources for optical communications and other optoelectronic applications.

Ultrafast frequency-agile terahertz devices using methylammonium lead halide perovskites

PubMed Central

Chanana, Ashish; Liu, Xiaojie; Vardeny, Zeev Valy

2018-01-01

The ability to control the response of metamaterial structures can facilitate the development of new terahertz devices, with applications in spectroscopy and communications. We demonstrate ultrafast frequency-agile terahertz metamaterial devices that enable such a capability, in which multiple perovskites can be patterned in each unit cell with micrometer-scale precision. To accomplish this, we developed a fabrication technique that shields already deposited perovskites from organic solvents, allowing for multiple perovskites to be patterned in close proximity. By doing so, we demonstrate tuning of the terahertz resonant response that is based not only on the optical pump fluence but also on the optical wavelength. Because polycrystalline perovskites have subnanosecond photocarrier recombination lifetimes, switching between resonances can occur on an ultrafast time scale. The use of multiple perovskites allows for new functionalities that are not possible using a single semiconducting material. For example, by patterning one perovskite in the gaps of split-ring resonators and bringing a uniform thin film of a second perovskite in close proximity, we demonstrate tuning of the resonant response using one optical wavelength and suppression of the resonance using a different optical wavelength. This general approach offers new capabilities for creating tunable terahertz devices. PMID:29736416

Spherical transceivers for ultrafast optical wireless communications

NASA Astrophysics Data System (ADS)

Jin, Xian; Hristovski, Blago A.; Collier, Christopher M.; Geoffroy-Gagnon, Simon; Born, Brandon; Holzman, Jonathan F.

2016-02-01

Optical wireless communications (OWC) offers the potential for high-speed and mobile operation in indoor networks. Such OWC systems often employ a fixed transmitter grid and mobile transceivers, with the mobile transceivers carrying out bi-directional communication via active downlinks (ideally with high-speed signal detection) and passive uplinks (ideally with broad angular retroreflection and high-speed modulation). It can be challenging to integrate all of these bidirectional communication capabilities within the mobile transceivers, however, as there is a simultaneous desire for compact packaging. With this in mind, the work presented here introduces a new form of transceiver for bi-directional OWC systems. The transceiver incorporates radial photoconductive switches (for high-speed signal detection) and a spherical retro-modulator (for broad angular retroreflection and high-speed all-optical modulation). All-optical retromodulation are investigated by way of theoretical models and experimental testing, for spherical retro-modulators comprised of three glasses, N-BK7, N-LASF9, and S-LAH79, having differing levels of refraction and nonlinearity. It is found that the spherical retro-modulator comprised of S-LAH79, with a refractive index of n ≍ 2 and a Kerr nonlinear index of n2 ≍ (1.8 ± 0.1) × 10-15 cm2/W, yields both broad angular retroreflection (over a solid angle of 2π steradians) and ultrafast modulation (over a duration of 120 fs). Such transceivers can become important elements for all-optical implementations in future bi-directional OWC systems.

Ultrafast Solvation Dynamics and Vibrational Coherences of Halogenated Boron-Dipyrromethene Derivatives Revealed through Two-Dimensional Electronic Spectroscopy.

PubMed

Lee, Yumin; Das, Saptaparna; Malamakal, Roy M; Meloni, Stephen; Chenoweth, David M; Anna, Jessica M

2017-10-18

Boron-dipyrromethene (BODIPY) chromophores have a wide range of applications, spanning areas from biological imaging to solar energy conversion. Understanding the ultrafast dynamics of electronically excited BODIPY chromophores could lead to further advances in these areas. In this work, we characterize and compare the ultrafast dynamics of halogenated BODIPY chromophores through applying two-dimensional electronic spectroscopy (2DES). Through our studies, we demonstrate a new data analysis procedure for extracting the dynamic Stokes shift from 2DES spectra revealing an ultrafast solvent relaxation. In addition, we extract the frequency of the vibrational modes that are strongly coupled to the electronic excitation, and compare the results of structurally different BODIPY chromophores. We interpret our results with the aid of DFT calculations, finding that structural modifications lead to changes in the frequency, identity, and magnitude of Franck-Condon active vibrational modes. We attribute these changes to differences in the electron density of the electronic states of the structurally different BODIPY chromophores.

All optical quantum control of a spin-quantum state and ultrafast transduction into an electric current.

PubMed

Müller, K; Kaldewey, T; Ripszam, R; Wildmann, J S; Bechtold, A; Bichler, M; Koblmüller, G; Abstreiter, G; Finley, J J

2013-01-01

The ability to control and exploit quantum coherence and entanglement drives research across many fields ranging from ultra-cold quantum gases to spin systems in condensed matter. Transcending different physical systems, optical approaches have proven themselves to be particularly powerful, since they profit from the established toolbox of quantum optical techniques, are state-selective, contact-less and can be extremely fast. Here, we demonstrate how a precisely timed sequence of monochromatic ultrafast (~ 2-5 ps) optical pulses, with a well defined polarisation can be used to prepare arbitrary superpositions of exciton spin states in a semiconductor quantum dot, achieve ultrafast control of the spin-wavefunction without an applied magnetic field and make high fidelity read-out the quantum state in an arbitrary basis simply by detecting a strong (~ 2-10 pA) electric current flowing in an external circuit. The results obtained show that the combined quantum state preparation, control and read-out can be performed with a near-unity (≥97%) fidelity.

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

Robust Stacking-Independent Ultrafast Charge Transfer in MoS2/WS2 Bilayers.

PubMed

Ji, Ziheng; Hong, Hao; Zhang, Jin; Zhang, Qi; Huang, Wei; Cao, Ting; Qiao, Ruixi; Liu, Can; Liang, Jing; Jin, Chuanhong; Jiao, Liying; Shi, Kebin; Meng, Sheng; Liu, Kaihui

2017-12-26

Van der Waals-coupled two-dimensional (2D) heterostructures have attracted great attention recently due to their high potential in the next-generation photodetectors and solar cells. The understanding of charge-transfer process between adjacent atomic layers is the key to design optimal devices as it directly determines the fundamental response speed and photon-electron conversion efficiency. However, general belief and theoretical studies have shown that the charge transfer behavior depends sensitively on interlayer configurations, which is difficult to control accurately, bringing great uncertainties in device designing. Here we investigate the ultrafast dynamics of interlayer charge transfer in a prototype heterostructure, the MoS 2 /WS 2 bilayer with various stacking configurations, by optical two-color ultrafast pump-probe spectroscopy. Surprisingly, we found that the charge transfer is robust against varying interlayer twist angles and interlayer coupling strength, in time scale of ∼90 fs. Our observation, together with atomic-resolved transmission electron characterization and time-dependent density functional theory simulations, reveals that the robust ultrafast charge transfer is attributed to the heterogeneous interlayer stretching/sliding, which provides additional channels for efficient charge transfer previously unknown. Our results elucidate the origin of transfer rate robustness against interlayer stacking configurations in optical devices based on 2D heterostructures, facilitating their applications in ultrafast and high-efficient optoelectronic and photovoltaic devices in the near future.

Ultrafast optical pulse convertor caused by oscillations of the energy level structure in the conjugated polymer poly(p-phenylenevinylene).

PubMed

Zhang, Yusong; Chen, Weikang; Lin, Zhe; Li, Sheng; George, Thomas F

2017-08-21

For a conjugated polymer irradiated by two optical pulses, the whole process of excitation, involving lattice oscillations, oscillations of the energy level structure, and evolution of the electron cloud, is investigated. Localization of the electron cloud appears in the first 100 fs of irradiation, which in turn induces vibrations of lattice of the polymer chain as well as oscillations of the band gap. These oscillations filter the absorption of the external optical field inversely and convert the original optical field to an ultrafast light field whose intensity varies with a certain period. Based on the mechanism, oscillations of the energy level structure, induced by the external excitation, can be designed as an ultrafast response optical convertor that is able to change the external optical pulse into a new effective light field with a certain oscillation period. This helps provide new insight into designing nanostructures for polymeric optoelectronics.

Ultrafast monoenergetic electron source by optical waveform control of surface plasmons.

PubMed

Dombi, Péter; Rácz, Péter

2008-03-03

We propose coherent control of photoelectron acceleration at metal surfaces mediated by surface plasmon polaritons. A high degree of spectral and spatial control of the emission process can be exercised by amplitude and phase controlling the optical waveform (including the carrier-envelope phase) of the plasmon generating few-cycle laser pulse. Numerical results show that the emitted electron beam is highly directional and monoenergetic suggesting applications in contemporary ultrafast methods where ultrashort, well-behaved electron pulses are required.

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).

Ultrafast light matter interaction in CdSe/ZnS core-shell quantum dots

NASA Astrophysics Data System (ADS)

Yadav, Rajesh Kumar; Sharma, Rituraj; Mondal, Anirban; Adarsh, K. V.

2018-04-01

Core-shell quantum dot are imperative for carrier (electron and holes) confinement in core/shell, which provides a stage to explore the linear and nonlinear optical phenomena at the nanoscalelimit. Here we present a comprehensive study of ultrafast excitation dynamics and nonlinear optical absorption of CdSe/ZnS core shell quantum dot with the help of ultrafast spectroscopy. Pump-probe and time-resolved measurements revealed the drop of trapping at CdSe surface due to the presence of the ZnS shell, which makes more efficient photoluminescence. We have carried out femtosecond transient absorption studies of the CdSe/ZnS core-shell quantum dot by irradiation with 400 nm laser light, monitoring the transients in the visible region. The optical nonlinearity of the core-shell quantum dot studied by using the Z-scan technique with 120 fs pulses at the wavelengths of 800 nm. The value of two photon absorption coefficients (β) of core-shell QDs extracted as80cm/GW, and it shows excellent benchmark for the optical limiting onset of 2.5GW/cm2 with the low limiting differential transmittance of 0.10, that is an order of magnitude better than graphene based materials.

High-yield, ultrafast, surface plasmon-enhanced, Au nanorod optical field electron emitter arrays.

PubMed

Hobbs, Richard G; Yang, Yujia; Fallahi, Arya; Keathley, Philip D; De Leo, Eva; Kärtner, Franz X; Graves, William S; Berggren, Karl K

2014-11-25

Here we demonstrate the design, fabrication, and characterization of ultrafast, surface-plasmon enhanced Au nanorod optical field emitter arrays. We present a quantitative study of electron emission from Au nanorod arrays fabricated by high-resolution electron-beam lithography and excited by 35 fs pulses of 800 nm light. We present accurate models for both the optical field enhancement of Au nanorods within high-density arrays, and electron emission from those nanorods. We have also studied the effects of surface plasmon damping induced by metallic interface layers at the substrate/nanorod interface on near-field enhancement and electron emission. We have identified the peak optical field at which the electron emission mechanism transitions from a 3-photon absorption mechanism to strong-field tunneling emission. Moreover, we have investigated the effects of nanorod array density on nanorod charge yield, including measurement of space-charge effects. The Au nanorod photocathodes presented in this work display 100-1000 times higher conversion efficiency relative to previously reported UV triggered emission from planar Au photocathodes. Consequently, the Au nanorod arrays triggered by ultrafast pulses of 800 nm light in this work may outperform equivalent UV-triggered Au photocathodes, while also offering nanostructuring of the electron pulse produced from such a cathode, which is of interest for X-ray free-electron laser (XFEL) development where nanostructured electron pulses may facilitate more efficient and brighter XFEL radiation.

Attosecond electron pulse trains and quantum state reconstruction in ultrafast transmission electron microscopy

NASA Astrophysics Data System (ADS)

Priebe, Katharina E.; Rathje, Christopher; Yalunin, Sergey V.; Hohage, Thorsten; Feist, Armin; Schäfer, Sascha; Ropers, Claus

2017-12-01

Ultrafast electron and X-ray imaging and spectroscopy are the basis for an ongoing revolution in the understanding of dynamical atomic-scale processes in matter. The underlying technology relies heavily on laser science for the generation and characterization of ever shorter pulses. Recent findings suggest that ultrafast electron microscopy with attosecond-structured wavefunctions may be feasible. However, such future technologies call for means to both prepare and fully analyse the corresponding free-electron quantum states. Here, we introduce a framework for the preparation, coherent manipulation and characterization of free-electron quantum states, experimentally demonstrating attosecond electron pulse trains. Phase-locked optical fields coherently control the electron wavefunction along the beam direction. We establish a new variant of quantum state tomography—`SQUIRRELS'—for free-electron ensembles. The ability to tailor and quantitatively map electron quantum states will promote the nanoscale study of electron-matter entanglement and new forms of ultrafast electron microscopy down to the attosecond regime.

Real-Time Observation of Internal Motion within Ultrafast Dissipative Optical Soliton Molecules

NASA Astrophysics Data System (ADS)

Krupa, Katarzyna; Nithyanandan, K.; Andral, Ugo; Tchofo-Dinda, Patrice; Grelu, Philippe

2017-06-01

Real-time access to the internal ultrafast dynamics of complex dissipative optical systems opens new explorations of pulse-pulse interactions and dynamic patterns. We present the first direct experimental evidence of the internal motion of a dissipative optical soliton molecule generated in a passively mode-locked erbium-doped fiber laser. We map the internal motion of a soliton pair molecule by using a dispersive Fourier-transform imaging technique, revealing different categories of internal pulsations, including vibrationlike and phase drifting dynamics. Our experiments agree well with numerical predictions and bring insights to the analogy between self-organized states of lights and states of the matter.

Transient and stationary spectroscopy of cytochrome c: ultrafast internal conversion controls photoreduction.

PubMed

Löwenich, Dennis; Kleinermanns, Karl; Karunakaran, Venugopal; Kovalenko, Sergey Alexander

2008-01-01

Photoreduction of cytochrome c (Cyt c) has been reinvestigated using femtosecond-to-nanosecond transient absorption and stationary spectroscopy. Femtosecond spectra of oxidized Cyt c, recorded in the probe range 270-1000 nm, demonstrate similar evolution upon 266 or 403 nm excitation: an ultrafast 0.3 ps internal conversion followed by a 4 ps vibrational cooling. Late transient spectra after 20 ps, from the cold ground-state chromophore, reveal a small but measurable signal from reduced Cyt c. The yield phi for Fe3+-->Fe2+ photoreduction is measured to be phi(403) = 0.016 and phi(266) = 0.08 for 403 and 266 nm excitation. These yields lead to a guess of the barrier E(f)(A) = 55 kJ mol(-1) for thermal ground-state electron transfer (ET). Nanosecond spectra initially show the typical absorption from reduced Cyt c and then exhibit temperature-dependent sub-microsecond decays (0.5 micros at 297 K), corresponding to a barrier E(A)(b) = 33 kJ mol(-1) for the back ET reaction and a reaction energy DeltaE = 22 kJ mol(-1). The nanosecond transients do not decay to zero on a second time scale, demonstrating the stability of some of the reduced Cyt c. The yields calculated from this stable reduced form agree with quasistationary reduction yields. Modest heating of Cyt c leads to its efficient thermal reduction as demonstrated by differential stationary absorption spectroscopy. In summary, our results point to ultrafast internal conversion of oxidized Cyt c upon UV or visible excitation, followed by Fe-porphyrin reduction due to thermal ground-state ET as the prevailing mechanism.

Applications of ultrafast laser direct writing: from polarization control to data storage

NASA Astrophysics Data System (ADS)

Donko, A.; Gertus, T.; Brambilla, G.; Beresna, M.

2018-02-01

Ultrafast laser direct writing is a fascinating technology which emerged more than two decades from fundamental studies of material resistance to high-intensity optical fields. Its development saw the discovery of many puzzling phenomena and demonstration of useful applications. Today, ultrafast laser writing is seen as a technology with great potential and is rapidly entering the industrial environment. Whereas, less than 10 years ago, ultrafast lasers were still confined within the research labs. This talk will overview some of the unique features of ultrafast lasers and give examples of its applications in optical data storage, polarization control and optical fibers.

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.

Excited state dynamics & optical control of molecular motors

NASA Astrophysics Data System (ADS)

Wiley, Ted; Sension, Roseanne

2014-03-01

Chiral overcrowded alkenes are likely candidates for light driven rotary molecular motors. At their core, these molecular motors are based on the chromophore stilbene, undergoing ultrafast cis/trans photoisomerization about their central double bond. Unlike stilbene, the photochemistry of molecular motors proceeds in one direction only. This unidirectional rotation is a result of helicity in the molecule induced by steric hindrance. However, the steric hindrance which ensures unidirectional excited state rotation, has the unfortunate consequence of producing large ground state barriers which dramatically decrease the overall rate of rotation. These molecular scale ultrafast motors have only recently been studied by ultrafast spectroscopy. Our lab has studied the photochemistry and photophysics of a ``first generation'' molecular motor with UV-visible transient absorption spectroscopy. We hope to use optical pulse shaping to enhance the efficiency and turnover rate of these molecular motors.

Ultrafast optical modification of exchange interactions in iron oxides

NASA Astrophysics Data System (ADS)

Mikhaylovskiy, R. V.; Hendry, E.; Secchi, A.; Mentink, J. H.; Eckstein, M.; Wu, A.; Pisarev, R. V.; Kruglyak, V. V.; Katsnelson, M. I.; Rasing, Th.; Kimel, A. V.

2015-09-01

Ultrafast non-thermal manipulation of magnetization by light relies on either indirect coupling of the electric field component of the light with spins via spin-orbit interaction or direct coupling between the magnetic field component and spins. Here we propose a scenario for coupling between the electric field of light and spins via optical modification of the exchange interaction, one of the strongest quantum effects with strength of 103 Tesla. We demonstrate that this isotropic opto-magnetic effect, which can be called inverse magneto-refraction, is allowed in a material of any symmetry. Its existence is corroborated by the experimental observation of terahertz emission by spin resonances optically excited in a broad class of iron oxides with a canted spin configuration. From its strength we estimate that a sub-picosecond modification of the exchange interaction by laser pulses with fluence of about 1 mJ cm-2 acts as a pulsed effective magnetic field of 0.01 Tesla.

Ultrafast optical modification of exchange interactions in iron oxides

PubMed Central

Mikhaylovskiy, R.V.; Hendry, E.; Secchi, A.; Mentink, J.H.; Eckstein, M.; Wu, A.; Pisarev, R.V.; Kruglyak, V.V.; Katsnelson, M.I.; Rasing, Th.; Kimel, A.V.

2015-01-01

Ultrafast non-thermal manipulation of magnetization by light relies on either indirect coupling of the electric field component of the light with spins via spin-orbit interaction or direct coupling between the magnetic field component and spins. Here we propose a scenario for coupling between the electric field of light and spins via optical modification of the exchange interaction, one of the strongest quantum effects with strength of 103 Tesla. We demonstrate that this isotropic opto-magnetic effect, which can be called inverse magneto-refraction, is allowed in a material of any symmetry. Its existence is corroborated by the experimental observation of terahertz emission by spin resonances optically excited in a broad class of iron oxides with a canted spin configuration. From its strength we estimate that a sub-picosecond modification of the exchange interaction by laser pulses with fluence of about 1 mJ cm−2 acts as a pulsed effective magnetic field of 0.01 Tesla. PMID:26373688

Ultrafast optical modification of exchange interactions in iron oxides.

PubMed

Mikhaylovskiy, R V; Hendry, E; Secchi, A; Mentink, J H; Eckstein, M; Wu, A; Pisarev, R V; Kruglyak, V V; Katsnelson, M I; Rasing, Th; Kimel, A V

2015-09-16

Ultrafast non-thermal manipulation of magnetization by light relies on either indirect coupling of the electric field component of the light with spins via spin-orbit interaction or direct coupling between the magnetic field component and spins. Here we propose a scenario for coupling between the electric field of light and spins via optical modification of the exchange interaction, one of the strongest quantum effects with strength of 10(3) Tesla. We demonstrate that this isotropic opto-magnetic effect, which can be called inverse magneto-refraction, is allowed in a material of any symmetry. Its existence is corroborated by the experimental observation of terahertz emission by spin resonances optically excited in a broad class of iron oxides with a canted spin configuration. From its strength we estimate that a sub-picosecond modification of the exchange interaction by laser pulses with fluence of about 1 mJ cm(-2) acts as a pulsed effective magnetic field of 0.01 Tesla.

White light Z-scan measurements of ultrafast optical nonlinearity in reduced graphene oxide nanosheets in the 400–700 nm region

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

Perumbilavil, Sreekanth; Sankar, Pranitha; Priya Rose, T.

Wavelength dispersion of optical power limiting is an important factor to be considered while designing potential optical limiters for laser safety applications. We report the observation of broadband, ultrafast optical limiting in reduced graphene oxide (rGO), measured by a single open aperture Z-scan using a white light continuum (WLC) source. WLC Z-scan is fast when the nonlinearity is to be measured over broad wavelength ranges, and it obviates the need for an ultrafast tunable laser making it cost-economic compared to conventional Z-scan. The nonlinearity arises from nondegenerate two-photon absorption, owing mostly to the crystallinity and extended π conjugation of rGO.

Experimental station for ultrafast extreme ultraviolet spectroscopy for non-equilibrium dynamics in warm dense matter

NASA Astrophysics Data System (ADS)

Lee, Jong-won; Geng, Xiaotao; Jung, Jae Hyung; Cho, Min Sang; Yang, Seong Hyeok; Jo, Jawon; Lee, Chang-lyoul; Cho, Byoung Ick; Kim, Dong-Eon

2018-07-01

Recent interest in highly excited matter generated by intense femtosecond laser pulses has led to experimental methods that directly investigate ultrafast non-equilibrium electronic and structural dynamics. We present a tabletop experimental station for the extreme ultraviolet (EUV) spectroscopy used to trace L-edge dynamics in warm dense aluminum with a temporal resolution of a hundred femtoseconds. The system consists of the EUV probe generation part via a high-order harmonic generation process of femtosecond laser pulses with atomic clusters, a beamline with high-throughput optics and a sample-refreshment system of nano-foils utilizing the full repetition rate of the probe, and a flat-field EUV spectrograph. With the accumulation of an order of a hundred shots, a clear observation of the change in the aluminum L-shell absorption was achieved with a temporal resolution of 90 fs in a 600-fs window. The signature of a non-equilibrium electron distribution over a 10-eV range and its evolution to a 1-eV Fermi distribution are observed. This demonstrates the capability of this apparatus to capture the non-equilibrium electron-hole dynamics in highly excited warm dense matter conditions.

THz Acoustic Spectroscopy by using Double Quantum Wells and Ultrafast Optical Spectroscopy.

PubMed

Wei, Fan Jun; Yeh, Yu-Hsiang; Sheu, Jinn-Kong; Lin, Kung-Hsuan

2016-06-27

GaN is a pivotal material for acoustic transducers and acoustic spectroscopy in the THz regime, but its THz phonon properties have not been experimentally and comprehensively studied. In this report, we demonstrate how to use double quantum wells as a THz acoustic transducer for measuring generated acoustic phonons and deriving a broadband acoustic spectrum with continuous frequencies. We experimentally investigated the sub-THz frequency dependence of acoustic attenuation (i.e., phonon mean-free paths) in GaN, in addition to its physical origins such as anharmonic scattering, defect scattering, and boundary scattering. A new upper limit of attenuation caused by anharmonic scattering, which is lower than previously reported values, was obtained. Our results should be noteworthy for THz acoustic spectroscopy and for gaining a fundamental understanding of heat conduction.

Material processing with fiber based ultrafast pulse delivery

NASA Astrophysics Data System (ADS)

Baumbach, S.; Stockburger, R.; Führa, B.; Zoller, S.; Thum, S.; Moosmann, J.; Maier, D.; Kanal, F.; Russ, S.; Kaiser, E.; Budnicki, A.; Sutter, D. H.; Pricking, S.; Killi, A.

2018-02-01

We report on TRUMPF's ultrafast laser systems equipped with industrialized hollow core fiber laser light cables. Beam guidance in general by means of optical fibers, e.g. for multi kilowatt cw laser systems, has become an integral part of laser-based material processing. One advantage of fiber delivery, among others, is the mechanical separation between laser and processing head. An equally important benefit is given by the fact that the fiber end acts as an opto-mechanical fix-point close to successive optical elements in the processing head. Components like lenses, diffractive optical elements etc. can thus be designed towards higher efficiency which results in better material processing. These aspects gain increasing significance when the laser system operates in fundamental mode which is usually the case for ultrafast lasers. Through the last years beam guidance of ultrafast laser pulses by means of hollow core fiber technology established very rapidly. The combination of TRUMPF's long-term stable ultrafast laser sources, passive fiber coupling, connector and packaging forms a flexible and powerful system for laser based material processing well suited for an industrial environment. In this article we demonstrate common material processing applications with ultrafast lasers realized with TRUMPF's hollow core fiber delivery. The experimental results are contrasted and evaluated against conventional free space propagation in order to illustrate the performance of flexible ultrafast beam delivery.

System and method for ultrafast optical signal detecting via a synchronously coupled anamorphic light pulse encoded laterally

DOEpatents

Heebner, John E [Livermore, CA

2010-08-03

In one general embodiment, a method for ultrafast optical signal detecting is provided. In operation, a first optical input signal is propagated through a first wave guiding layer of a waveguide. Additionally, a second optical input signal is propagated through a second wave guiding layer of the waveguide. Furthermore, an optical control signal is applied to a top of the waveguide, the optical control signal being oriented diagonally relative to the top of the waveguide such that the application is used to influence at least a portion of the first optical input signal propagating through the first wave guiding layer of the waveguide. In addition, the first and the second optical input signals output from the waveguide are combined. Further, the combined optical signals output from the waveguide are detected. In another general embodiment, a system for ultrafast optical signal recording is provided comprising a waveguide including a plurality of wave guiding layers, an optical control source positioned to propagate an optical control signal towards the waveguide in a diagonal orientation relative to a top of the waveguide, at least one optical input source positioned to input an optical input signal into at least a first and a second wave guiding layer of the waveguide, and a detector for detecting at least one interference pattern output from the waveguide, where at least one of the interference patterns results from a combination of the optical input signals input into the first and the second wave guiding layer. Furthermore, propagation of the optical control signal is used to influence at least a portion of the optical input signal propagating through the first wave guiding layer of the waveguide.

An innovative Yb-based ultrafast deep ultraviolet source for time-resolved photoemission experiments

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

Boschini, F.; Hedayat, H.; Dallera, C.

2014-12-15

Time- and angle-resolved photoemission spectroscopy is a powerful technique to study ultrafast electronic dynamics in solids. Here, an innovative optical setup based on a 100-kHz Yb laser source is presented. Exploiting non-collinear optical parametric amplification and sum-frequency generation, ultrashort pump (hν = 1.82 eV) and ultraviolet probe (hν = 6.05 eV) pulses are generated. Overall temporal and instrumental energy resolutions of, respectively, 85 fs and 50 meV are obtained. Time- and angle-resolved measurements on BiTeI semiconductor are presented to show the capabilities of the setup.

A study of the proteorhodopsin primary photoreaction by low-temperature FTIR difference and ultrafast transient infrared spectroscopy

NASA Astrophysics Data System (ADS)

Amsden, Jason J.

Proteorhodopsin (PR), a newly discovered microbial rhodopsin found in marine proteobacteria, functions as a light-driven proton pump similar to bacteriorhodopsin (BR). PR-containing bacteria account for ˜13% of the microorganisms in the oceans' photic zone and are responsible for a significant fraction of the biosphere's solar energy conversion. We study the initial response of proteorhodopsin to photon absorption using a combination of low-temperature (80 K) Fourier transform infrared (FTIR) difference spectroscopy and ultrafast transient infrared (TIR) spectroscopy. Low-temperature FTIR difference spectroscopy combined with site-directed mutagenesis and isotope labeling is used to detect and characterize changes occurring in the conformation of the retinal chromophore, protein, and internal water molecules of green-absorbing PR (GPR) and blue-absorbing PR (BPR) during the initial phototransition. Measurements on cryogenically trapped intermediates do not accurately reflect all native structural changes occurring in PR and other microbial rhodopsins on ultrafast time scales at room temperature. Recent studies demonstrate that photoactive proteins such as photoactive yellow protein, myoglobin, and green-fluorescent protein, can react within several picoseconds to photon absorption by their chromophores. Faster subpicosecond protein responses have been suggested to occur in rhodopsin-like proteins where retinal chromophore photoisomerization may impulsively drive structural changes in nearby protein groups. Here, I test this possibility by investigating the earliest protein and chromophore structural changes occurring in GPR using ultrafast TIR spectroscopy with ˜200 fs time resolution combined with non-perturbing isotope labeling. On the basis of total-15N and retinal C15D (retinal with a deuterium on carbon 15) isotope labeling, the all-trans to 13-cis retinal chromophore isomerization occurs with a 500-700 fs time constant and the amide II mode of one or more

Ultrafast carrier dynamics and optical pumping of lasing from Ar-plasma treated ZnO nanoribbons

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

Sarkar, Ketaki; Mukherjee, Souvik; Wiederrecht, Gary

We report that it is a well-known fact that ZnO has been one of the most studied wide bandgap II-VI materials by the scientific community specifically due to its potential for being used as exciton-related optical devices. Hence, realizing ways to increase the efficiency of these devices is important. We discuss a plasma treatment technique to enhance the near-band-edge (NBE) excitonic emission from ZnO based nanoribbons. We observed an enhancement of the NBE peak and simultaneous quenching of the visible emission peak resulting from the removal of surface traps on these ZnO nanoribbons. More importantly, we report here the associatedmore » ultrafast carrier dynamics resulting from this surface treatment. Femtosecond transient absorption spectroscopy was performed using pump-probe differential transmission measurements shedding new light on these improved dynamics with faster relaxation times. The knowledge obtained is important for improving the application of ZnO based optoelectronic devices. Finally, we also observed how these improved carrier dynamics have a direct effect on the threshold and efficiency of random lasing from the material.« less

Ultrafast carrier dynamics and optical pumping of lasing from Ar-plasma treated ZnO nanoribbons

DOE PAGES

Sarkar, Ketaki; Mukherjee, Souvik; Wiederrecht, Gary; ...

2018-01-04

We report that it is a well-known fact that ZnO has been one of the most studied wide bandgap II-VI materials by the scientific community specifically due to its potential for being used as exciton-related optical devices. Hence, realizing ways to increase the efficiency of these devices is important. We discuss a plasma treatment technique to enhance the near-band-edge (NBE) excitonic emission from ZnO based nanoribbons. We observed an enhancement of the NBE peak and simultaneous quenching of the visible emission peak resulting from the removal of surface traps on these ZnO nanoribbons. More importantly, we report here the associatedmore » ultrafast carrier dynamics resulting from this surface treatment. Femtosecond transient absorption spectroscopy was performed using pump-probe differential transmission measurements shedding new light on these improved dynamics with faster relaxation times. The knowledge obtained is important for improving the application of ZnO based optoelectronic devices. Finally, we also observed how these improved carrier dynamics have a direct effect on the threshold and efficiency of random lasing from the material.« less

Ultrafast X-Ray Absorption Spectroscopy of Isochorically Heated Warm Dense Matter

NASA Astrophysics Data System (ADS)

Engelhorn, Kyle Craig

This dissertation will present a series of new tools, together with new techniques, focused on the understanding of warm and dense matter. We report on the development of a high time resolution and high detection efficiency x-ray camera. The camera is integrated with a short pulse laser and an x-ray beamline at the Advanced Light Source synchrotron. This provides an instrument for single shot, broadband x-ray absorption spectroscopy of warm and dense matter with 2 picosecond time resolution. Warm and dense matter is created by isochorically heating samples of known density with an ultrafast optical laser pulse, and X-ray absorption spectroscopy probes the unoccupied electronic density of states before the onset of hydrodynamic expansion and electron-ion equilibrium is reached. Measured spectra from a variety of materials are compared with first principle molecular dynamics and density functional theory calculations. In heated silicon dioxide spectra, two novel pre-edge features are observed, a peak below the band gap and absorption within the band gap, while a reduction was observed in the features above the edge. From consideration of the calculated spectra, the peak below the gap is attributed to valence electrons that have been promoted to the conduction band, the absorption within the gap is attributed to broken Si-O bonds, and the reduction above the edge is attributed to an elevated ionic temperature. In heated copper spectra, a time-dependent shift and broadening of the absorption edge are observed, consistent with and elevated electron temperature. The temporal evolution of the electronic temperature is accurately determined by fitting the measured spectra with calculated spectra. The electron-ion equilibration is studied with a two-temperature model. In heated nickel spectra, a shift of the absorption edge is observed. This shift is found to be inconsistent with calculated spectra and independent of incident laser fluence. A shift of the chemical potential

Characterization of ultrafast devices using novel optical techniques

NASA Astrophysics Data System (ADS)

Ali, Md Ershad

Optical techniques have been extensively used to examine the high frequency performance of a number of devices including High Electron Mobility Transistors (HEMTs), Heterojunction Bipolar Phototransistors (HPTs) and Low Temperature GaAs (LT-GaAs) Photoconductive Switches. To characterize devices, frequency and time domain techniques, namely optical heterodyning and electro-optic sampling, having measurement bandwidths in excess of 200 GHz, were employed. Optical mixing in three-terminal devices has been extended for the first time to submillimeter wave frequencies. Using a new generation of 50-nm gate pseudomorphic InP-based HEMTs, optically mixed signals were detected to 552 GHz with a signal-to-noise ratio of approximately 5 dB. To the best of our knowledge, this is the highest frequency optical mixing obtained in three- terminal devices to date. A novel harmonic three-wave detection scheme was used for the detection of the optically generated signals. The technique involved downconversion of the signal in the device by the second harmonic of a gate-injected millimeter wave local oscillator. Measurements were also conducted up to 212 GHz using direct optical mixing and up to 382 GHz using a fundamental three-wave detection scheme. New interesting features in the bias dependence of the optically mixed signals have been reported. An exciting novel development from this work is the successful integration of near-field optics with optical heterodyning. The technique, called near-field optical heterodyning (NFOH), allows for extremely localized injection of high-frequency stimulus to any arbitrary point of an ultrafast device or circuit. Scanning the point of injection across the sample provides details of the high frequency operation of the device with high spatial resolution. For the implementation of the technique, fiber-optic probes with 100 nm apertures were fabricated. A feedback controlled positioning system was built for accurate placement and scanning of the

Supercomputations and big-data analysis in strong-field ultrafast optical physics: filamentation of high-peak-power ultrashort laser pulses

NASA Astrophysics Data System (ADS)

Voronin, A. A.; Panchenko, V. Ya; Zheltikov, A. M.

2016-06-01

High-intensity ultrashort laser pulses propagating in gas media or in condensed matter undergo complex nonlinear spatiotemporal evolution where temporal transformations of optical field waveforms are strongly coupled to an intricate beam dynamics and ultrafast field-induced ionization processes. At the level of laser peak powers orders of magnitude above the critical power of self-focusing, the beam exhibits modulation instabilities, producing random field hot spots and breaking up into multiple noise-seeded filaments. This problem is described by a (3  +  1)-dimensional nonlinear field evolution equation, which needs to be solved jointly with the equation for ultrafast ionization of a medium. Analysis of this problem, which is equivalent to solving a billion-dimensional evolution problem, is only possible by means of supercomputer simulations augmented with coordinated big-data processing of large volumes of information acquired through theory-guiding experiments and supercomputations. Here, we review the main challenges of supercomputations and big-data processing encountered in strong-field ultrafast optical physics and discuss strategies to confront these challenges.

Ultrafast control and monitoring of material properties using terahertz pulses

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

Bowlan, Pamela Renee

These are a set of slides on ultrafast control and monitoring of material properties using terahertz pulses. A few of the topics covered in these slides are: How fast is a femtosecond (fs), Different frequencies probe different properties of molecules or solids, What can a THz pulse do to a material, Ultrafast spectroscopy, Generating and measuring ultrashort THz pulses, Tracking ultrafast spin dynamics in antiferromagnets through spin wave resonances, Coherent two-dimensional THz spectroscopy, and Probing vibrational dynamics at a surface. Conclusions are: Coherent two-dimensional THz spectroscopy: a powerful approach for studying coherence and dynamics of low energy resonances. Applying thismore » to graphene we investigated the very strong THz light mater interaction which dominates over scattering. Useful for studying coupled excitations in multiferroics and monitoring chemical reactions. Also, THz-pump, SHG-probe spectoscopy: an ultrafast, surface sensitive probe of atomic-scale symmetry changes and nonlinear phonon dymanics. We are using this in Bi 2Se 3 to investigate the nonlinear surface phonon dynamics. This is potentially very useful for studying catalysis.« less

Ultrafast spontaneous emission of copper-doped silicon enhanced by an optical nanocavity.

PubMed

Sumikura, Hisashi; Kuramochi, Eiichi; Taniyama, Hideaki; Notomi, Masaya

2014-05-23

Dopants in silicon (Si) have attracted attention in the fields of photonics and quantum optics. However, the optical characteristics are limited by the small spontaneous emission rate of dopants in Si. This study demonstrates a large increase in the spontaneous emission rate of copper isoelectronic centres (Cu-IECs) doped into Si photonic crystal nanocavities. In a cavity with a quality factor (Q) of ~16,000, the photoluminescence (PL) lifetime of the Cu-IECs is 1.1 ns, which is 30 times shorter than the lifetime of a sample without a cavity. The PL decay rate is increased in proportion to Q/Vc (Vc is the cavity mode volume), which indicates the Purcell effect. This is the first demonstration of a cavity-enhanced ultrafast spontaneous emission from dopants in Si, and it may lead to the development of fast and efficient Si light emitters and Si quantum optical devices based on dopants with efficient optical access.

Ultrafast spontaneous emission of copper-doped silicon enhanced by an optical nanocavity

PubMed Central

SUMIKURA, HISASHI; KURAMOCHI, EIICHI; TANIYAMA, HIDEAKI; NOTOMI, MASAYA

2014-01-01

Dopants in silicon (Si) have attracted attention in the fields of photonics and quantum optics. However, the optical characteristics are limited by the small spontaneous emission rate of dopants in Si. This study demonstrates a large increase in the spontaneous emission rate of copper isoelectronic centres (Cu-IECs) doped into Si photonic crystal nanocavities. In a cavity with a quality factor (Q) of ~16,000, the photoluminescence (PL) lifetime of the Cu-IECs is 1.1 ns, which is 30 times shorter than the lifetime of a sample without a cavity. The PL decay rate is increased in proportion to Q/Vc (Vc is the cavity mode volume), which indicates the Purcell effect. This is the first demonstration of a cavity-enhanced ultrafast spontaneous emission from dopants in Si, and it may lead to the development of fast and efficient Si light emitters and Si quantum optical devices based on dopants with efficient optical access. PMID:24853336

On the relation between Marcus theory and ultrafast spectroscopy of solvation kinetics

NASA Astrophysics Data System (ADS)

Roy, Santanu; Galib, Mirza; Schenter, Gregory K.; Mundy, Christopher J.

2018-01-01

The phenomena of solvent exchange control the process of solvating ions, protons, and charged molecules. Building upon our extension of Marcus' philosophy of electron transfer, we provide a new perspective of ultrafast solvent exchange mechanism around ions measurable by two-dimensional infrared (2DIR) spectroscopy. In this theory, solvent rearrangement drives an ion-bound water to an activated state of higher coordination number, triggering ion-water separation that leads to the solvent-bound state of the water molecule. This ion-bound to solvent-bound transition rate for a BF4--water system is computed using ab initio molecular dynamics and Marcus theory, and is found to be in excellent agreement with the 2DIR measurement.

New Aspects of Photocurrent Generation at Graphene pn Junctions Revealed by Ultrafast Optical Measurements

NASA Astrophysics Data System (ADS)

Aivazian, Grant; Sun, Dong; Jones, Aaron; Ross, Jason; Yao, Wang; Cobden, David; Xu, Xiaodong

2012-02-01

The remarkable electrical and optical properties of graphene make it a promising material for new optoelectronic applications. However, one important, but so far unexplored, property is the role of hot carriers in charge and energy transport at graphene interfaces. Here we investigate the photocurrent (PC) dynamics at a tunable graphene pn junction using ultrafast scanning PC microscopy. Pump-probe measurements show a temperature dependent relaxation time of photogenerated carriers that increases from 1.5ps at 290K to 4ps at 20K; while the amplitude of the PC is independent of the lattice temperature. These observations imply that it is hot carriers, not phonons, which dominate ultrafast energy transport. Gate dependent measurements show many interesting features such as pump induced saturation, enhancement, and sign reversal of probe generated PC. These observations reveal that the underlying PC mechanism is a combination of the thermoelectric and built-in electric field effects. Our results enhance the understanding of non-equilibrium electron dynamics, electron-electron interactions, and electron-phonon interactions in graphene. They also determine fundamental limits on ultrafast device operation speeds (˜500 GHz) for graphene-based photodetectors.

Ultra-fast dynamics in the nonlinear optical response of silver nanoprism ordered arrays.

PubMed

Sánchez-Esquivel, Héctor; Raygoza-Sanchez, Karen Y; Rangel-Rojo, Raúl; Kalinic, Boris; Michieli, Niccolò; Cesca, Tiziana; Mattei, Giovanni

2018-03-15

In this work we present the study of the ultra-fast dynamics of the nonlinear optical response of a honeycomb array of silver triangular nanoprisms, performed using a femtosecond pulsed laser tuned with the dipolar surface plasmon resonance of the nanoarray. Nonlinear absorption and refraction, and their time-dependence, were explored using the z-scan and time-resolved excite-probe techniques. Nonlinear absorption is shown to change sign with the input irradiance and the behavior was explained on the basis of a three-level model. The response time was determined to be in the picosecond regime. A technique based on a variable frequency chopper was also used in order to discriminate the thermal and electronic contributions to the nonlinearity, which were found to have opposite signs. All these findings propel the investigated nanoprism arrays as good candidates for applications in advanced ultra-fast nonlinear nanophotonic devices.

Monitoring Ultrafast Chemical Dynamics by Time-Domain X-ray Photo- and Auger-Electron Spectroscopy.

PubMed

Gessner, Oliver; Gühr, Markus

2016-01-19

The directed flow of charge and energy is at the heart of all chemical processes. Extraordinary efforts are underway to monitor and understand the concerted motion of electrons and nuclei with ever increasing spatial and temporal sensitivity. The element specificity, chemical sensitivity, and temporal resolution of ultrafast X-ray spectroscopy techniques hold great promise to provide new insight into the fundamental interactions underlying chemical dynamics in systems ranging from isolated molecules to application-like devices. Here, we focus on the potential of ultrafast X-ray spectroscopy techniques based on the detection of photo- and Auger electrons to provide new fundamental insight into photochemical processes of systems with various degrees of complexity. Isolated nucleobases provide an excellent testing ground for our most fundamental understanding of intramolecular coupling between electrons and nuclei beyond the traditionally applied Born-Oppenheimer approximation. Ultrafast electronic relaxation dynamics enabled by the breakdown of this approximation is the major component of the nucleobase photoprotection mechanisms. Transient X-ray induced Auger electron spectroscopy on photoexcited thymine molecules provides atomic-site specific details of the extremely efficient coupling that converts potentially bond changing ultraviolet photon energy into benign heat. In particular, the time-dependent spectral shift of a specific Auger band is sensitive to the length of a single bond within the molecule. The X-ray induced Auger transients show evidence for an electronic transition out of the initially excited state within only ∼200 fs in contrast to theoretically predicted picosecond population trapping behind a reaction barrier. Photoinduced charge transfer dynamics between transition metal complexes and semiconductor nanostructures are of central importance for many emerging energy and climate relevant technologies. Numerous demonstrations of photovoltaic and

Large-area tungsten disulfide for ultrafast photonics.

PubMed

Yan, Peiguang; Chen, Hao; Yin, Jinde; Xu, Zihan; Li, Jiarong; Jiang, Zike; Zhang, Wenfei; Wang, Jinzhang; Li, Irene Ling; Sun, Zhipei; Ruan, Shuangchen

2017-02-02

Two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have attracted significant interest in various optoelectronic applications due to their excellent nonlinear optical properties. One of the most important applications of TMDs is to be employed as an extraordinary optical modulation material (e.g., the saturable absorber (SA)) in ultrafast photonics. The main challenge arises while embedding TMDs into fiber laser systems to generate ultrafast pulse trains and thus constraints their practical applications. Herein, few-layered WS 2 with a large-area was directly transferred on the facet of the pigtail and acted as a SA for erbium-doped fiber laser (EDFL) systems. In our study, WS 2 SA exhibited remarkable nonlinear optical properties (e.g., modulation depth of 15.1% and saturable intensity of 157.6 MW cm -2 ) and was used for ultrafast pulse generation. The soliton pulses with remarkable performances (e.g., ultrashort pulse duration of 1.49 ps, high stability of 71.8 dB, and large pulse average output power of 62.5 mW) could be obtained in a telecommunication band. To the best of our knowledge, the average output power of the mode-locked pulse trains is the highest by employing TMD materials in fiber laser systems. These results indicate that atomically large-area WS 2 could be used as excellent optical modulation materials in ultrafast photonics.

Time-resolved fluorescence and ultrafast energy transfer in a zinc (hydr)oxide-graphite oxide mesoporous composite

NASA Astrophysics Data System (ADS)

Secor, Jeff; Narinesingh, Veeshan; Seredych, Mykola; Giannakoudakis, Dimitrios A.; Bandosz, Teresa; Alfano, Robert R.

2015-01-01

Ultrafast energy decay kinetics of a zinc (hydr)oxide-graphite oxide (GO) composite is studied via time-resolved fluorescence spectroscopy. The time-resolved emission is spectrally decomposed into emission regions originating from the zinc (hydr)oxide optical gap, surface, and defect states of the composite material. The radiative lifetime of deep red emission becomes an order of magnitude longer than that of GO alone while the radiative lifetime of the zinc optical gap is shortened in the composite. An energy transfer scheme from the zinc (hydr)oxide to GO is considered.

Nonlinear-optical activity owing to anisotropy of ultrafast nonlinear refraction in cubic materials.

PubMed

Hutchings, D C

1995-08-01

The evolution of the polarization state in a cubic material with an anisotropic Kerr nonlinearity is examined. It is shown that in certain cases this provides a mechanism for nonlinear-optical activity, leaving the state of the polarization unchanged but causing a signif icant rotation in its major axis. The use of the anisotropic ultrafast nonlinear refraction that exists just beneath the half-gap in semiconductors to demonstrate these effects is discussed.

PREFACE: XVIII International Youth Scientific School "Coherent Optics and Optical Spectroscopy"

NASA Astrophysics Data System (ADS)

Salakhov, M. Kh; Samartsev, V. V.; Gainutdinov, R. Kh

2015-05-01

Kazan Federal University has held the annual International Youth School "Coherent Optics and Optical Spectroscopy" since 1997. The choice of the topic is not accidental. Kazan is the home of photon echo which was predicted at Kazan Physical-Technical Institute in 1963 by Prof. U.G. Kopvil'em and V.R. Nagibarov and observed in Columbia University by N.A. Kurnit, I.D. Abella, and S.R. Hartmann in 1964. Since then, photon echo has become a powerful tool of coherent optical spectroscopy and optical information processing, which have been developed here in Kazan in close collaboration between Kazan Physical-Technical Institute and Kazan Federal University. The main subjects of the XVIII International Youth School are: Nonlinear and coherent optics; Atomic and molecular spectroscopy; Coherent laser spectroscopy; Problems of quantum optics; Quantum theory of radiation; and Nanophotonics and Scanning Probe Microscopy. The unchallenged organizers of that school are Kazan Federal University and Kazan E.K. Zavoisky Physical-Technical Institute. The rector of the School is Professor Myakzyum Salakhov, and the vice-rector is Professor Vitaly Samartsev. The International Youth Scientific School "Coherent Optics and Optical Spectroscopy" follows the global pattern of comprehensive studies of matter properties and their interaction with electromagnetic fields. Since 1997 more than 100 famous scientists from the USA, Germany, Ukraine, Belarus and Russia have given plenary lecture presentations. Here over 1000 young scientists had an opportunity to participate in lively discussions about the latest scientific news. Many young people have submitted interesting reports on photonics, quantum electronics, laser physics, quantum optics, traditional optical and laser spectroscopy, non-linear optics, material science and nanotechnology. Here we are publishing the fullsize papers prepared from the most interesting lectures and reports selected by the Program Committee of the School. The

Measurement of ultrafast optical Kerr effect of Ge-Sb-Se chalcogenide slab waveguides by the beam self-trapping technique

NASA Astrophysics Data System (ADS)

Kuriakose, Tintu; Baudet, Emeline; Halenkovič, Tomáš; Elsawy, Mahmoud M. R.; Němec, Petr; Nazabal, Virginie; Renversez, Gilles; Chauvet, Mathieu

2017-11-01

We present a reliable and original experimental technique based on the analysis of beam self-trapping to measure ultrafast optical nonlinearities in planar waveguides. The technique is applied to the characterization of Ge-Sb-Se chalcogenide films that allow Kerr induced self-focusing and soliton formation. Linear and nonlinear optical constants of three different chalcogenide waveguides are studied at 1200 and 1550 nm in femtosecond regime. Waveguide propagation loss and two photon absorption coefficients are determined by transmission analysis. Beam broadening and narrowing results are compared with simulations of the nonlinear Schrödinger equation solved by BPM method to deduce the Kerr n2 coefficients. Kerr optical nonlinearities obtained by our original technique compare favorably with the values obtained by Z-scan technique. Nonlinear refractive index as high as (69 ± 11) × 10-18m2 / W is measured in Ge12.5Sb25Se62.5 at 1200 nm with low nonlinear absorption and low propagation losses which reveals the great characteristics of our waveguides for ultrafast all optical switching and integrated photonic devices.

Rapid and economical data acquisition in ultrafast frequency-resolved spectroscopy using choppers and a microcontroller.

PubMed

Guo, Liang; Monahan, Daniele M; Fleming, Graham

2016-08-08

Spectrometers and cameras are used in ultrafast spectroscopy to achieve high resolution in both time and frequency domains. Frequency-resolved signals from the camera pixels cannot be processed by common lock-in amplifiers, which have only a limited number of input channels. Here we demonstrate a rapid and economical method that achieves the function of a lock-in amplifier using mechanical choppers and a programmable microcontroller. We demonstrate the method's effectiveness by performing a frequency-resolved pump-probe measurement on the dye Nile Blue in solution.

Aqueye+: a new ultrafast single photon counter for optical high time resolution astrophysics

NASA Astrophysics Data System (ADS)

Zampieri, L.; Naletto, G.; Barbieri, C.; Verroi, E.; Barbieri, M.; Ceribella, G.; D'Alessandro, M.; Farisato, G.; Di Paola, A.; Zoccarato, P.

2015-05-01

Aqueye+ is a new ultrafast optical single photon counter, based on single photon avalanche photodiodes (SPAD) and a 4- fold split-pupil concept. It is a completely revisited version of its predecessor, Aqueye, successfully mounted at the 182 cm Copernicus telescope in Asiago. Here we will present the new technological features implemented on Aqueye+, namely a state of the art timing system, a dedicated and optimized optical train, a high sensitivity and high frame rate field camera and remote control, which will give Aqueye plus much superior performances with respect to its predecessor, unparalleled by any other existing fast photometer. The instrument will host also an optical vorticity module to achieve high performance astronomical coronography and a real time acquisition of atmospheric seeing unit. The present paper describes the instrument and its first performances.

Time of flight emission spectroscopy of laser produced nickel plasma: Short-pulse and ultrafast excitations

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

Smijesh, N.; Chandrasekharan, K.; Joshi, Jagdish C.

2014-07-07

We report the experimental investigation and comparison of the temporal features of short-pulse (7 ns) and ultrafast (100 fs) laser produced plasmas generated from a solid nickel target, expanding into a nitrogen background. When the ambient pressure is varied in a large range of 10⁻⁶Torr to 10²Torr, the plume intensity is found to increase rapidly as the pressure crosses 1 Torr. Time of flight (TOF) spectroscopy of emission from neutral nickel (Ni I) at 361.9 nm (3d⁹(²D) 4p → 3d⁹(²D) 4s transition) reveals two peaks (fast and slow species) in short-pulse excitation and a single peak in ultrafast excitation. Themore » fast and slow peaks represent recombined neutrals and un-ionized neutrals, respectively. TOF emission from singly ionized nickel (Ni II) studied using the 428.5 nm (3p⁶3d⁸(³P) 4s→ 3p⁶3d⁹ 4s) transition shows only a single peak for either excitation. Velocities of the neutral and ionic species are determined from TOF measurements carried out at different positions (i.e., at distances of 2 mm and 4 mm, respectively, from the target surface) on the plume axis. Measured velocities indicate acceleration of neutrals and ions, which is caused by the Coulomb pull of the electrons enveloping the plume front in the case of ultrafast excitation. Both Coulomb pull and laser-plasma interaction contribute to the acceleration in the case of short-pulse excitation. These investigations provide new information on the pressure dependent temporal behavior of nickel plasmas produced by short-pulse and ultrafast laser pulses, which have potential uses in applications such as pulsed laser deposition and laser-induced nanoparticle generation.« less

Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells

PubMed Central

Vella, Eleonora; Li, Hao; Grégoire, Pascal; Tuladhar, Sachetan M.; Vezie, Michelle S.; Few, Sheridan; Bazán, Claudia M.; Nelson, Jenny; Silva-Acuña, Carlos; Bittner, Eric R.

2016-01-01

All-organic-based photovoltaic solar cells have attracted considerable attention because of their low-cost processing and short energy payback time. In such systems the primary dissociation of an optical excitation into a pair of photocarriers has been recently shown to be extremely rapid and efficient, but the physical reason for this remains unclear. Here, two-dimensional photocurrent excitation spectroscopy, a novel non-linear optical spectroscopy, is used to probe the ultrafast coherent decay of photoexcitations into charge-producing states in a polymer:fullerene based solar cell. The two-dimensional photocurrent spectra are interpreted by introducing a theoretical model for the description of the coupling of the electronic states of the system to an external environment and to the applied laser fields. The experimental data show no cross-peaks in the twodimensional photocurrent spectra, as predicted by the model for coherence times between the exciton and the photocurrent producing states of 20 fs or less. PMID:27412119

Photogenerated Intrinsic Free Carriers in Small-molecule Organic Semiconductors Visualized by Ultrafast Spectroscopy

PubMed Central

He, Xiaochuan; Zhu, Gangbei; Yang, Jianbing; Chang, Hao; Meng, Qingyu; Zhao, Hongwu; Zhou, Xin; Yue, Shuai; Wang, Zhuan; Shi, Jinan; Gu, Lin; Yan, Donghang; Weng, Yuxiang

2015-01-01

Confirmation of direct photogeneration of intrinsic delocalized free carriers in small-molecule organic semiconductors has been a long-sought but unsolved issue, which is of fundamental significance to its application in photo-electric devices. Although the excitonic description of photoexcitation in these materials has been widely accepted, this concept is challenged by recently reported phenomena. Here we report observation of direct delocalized free carrier generation upon interband photoexcitation in highly crystalline zinc phthalocyanine films prepared by the weak epitaxy growth method using ultrafast spectroscopy. Transient absorption spectra spanning the visible to mid-infrared region revealed the existence of short-lived free electrons and holes with a diffusion length estimated to cross at least 11 molecules along the π−π stacking direction that subsequently localize to form charge transfer excitons. The interband transition was evidenced by ultraviolet-visible absorption, photoluminescence and electroluminescence spectroscopy. Our results suggest that delocalized free carriers photogeneration can also be achieved in organic semiconductors when the molecules are packed properly. PMID:26611323

Confocal ultrafast pump-probe spectroscopy: a new technique to explore nanoscale composites.

PubMed

Virgili, Tersilla; Grancini, Giulia; Molotokaite, Egle; Suarez-Lopez, Inma; Rajendran, Sai Kiran; Liscio, Andrea; Palermo, Vincenzo; Lanzani, Guglielmo; Polli, Dario; Cerullo, Giulio

2012-04-07

This article is devoted to the exploration of the benefits of a new ultrafast confocal pump-probe technique, able to study the photophysics of different structured materials with nanoscale resolution. This tool offers many advantages over standard stationary microscopy techniques because it directly interrogates excited state dynamics in molecules, providing access to both radiative and non-radiative deactivation processes at a local scale. In this paper we present a few different examples of its application to organic semiconductor systems. The first two are focussed on the study of the photophysics of phase-separated polymer blends: (i) a blue-emitting polyfluorene (PFO) in an inert matrix of PMMA and (ii) an electron donor polythiophene (P3HT) mixed with an electron acceptor fullerene derivative (PCBM). The experimental results on these samples demonstrate the capability of the technique to unveil peculiar interfacial dynamics at the border region between phase-segregated domains, which would be otherwise averaged out using conventional pump-probe spectroscopy. The third example is the study of the photophysics of isolated mesoscopic crystals of the PCBM molecule. Our ultrafast microscope could evidence the presence of two distinctive regions within the crystals. In particular, we could pinpoint for the first time areas within the crystals showing photobleaching/stimulated emission signals from a charge-transfer state. This journal is © The Royal Society of Chemistry 2012

Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources

DOE PAGES

Roseker, W.; Hruszkewycz, S. O.; Lehmkuhler, F.; ...

2018-04-27

One of the important challenges in condensed matter science is to understand ultrafast, atomic-scale fluctuations that dictate dynamic processes in equilibrium and non-equilibrium materials. Here, we report an important step towards reaching that goal by using a state-of-the-art perfect crystal based split-and-delay system, capable of splitting individual X-ray pulses and introducing femtosecond to nanosecond time delays. We show the results of an ultrafast hard X-ray photon correlation spectroscopy experiment at LCLS where split X-ray pulses were used to measure the dynamics of gold nanoparticles suspended in hexane. We show how reliable speckle contrast values can be extracted even from verymore » low intensity free electron laser (FEL) speckle patterns by applying maximum likelihood fitting, thus demonstrating the potential of a split-and-delay approach for dynamics measurements at FEL sources. This will enable the characterization of equilibrium and, importantly also reversible non-equilibrium processes in atomically disordered materials.« less

Towards ultrafast dynamics with split-pulse X-ray photon correlation spectroscopy at free electron laser sources

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

Roseker, W.; Hruszkewycz, S. O.; Lehmkuhler, F.

One of the important challenges in condensed matter science is to understand ultrafast, atomic-scale fluctuations that dictate dynamic processes in equilibrium and non-equilibrium materials. Here, we report an important step towards reaching that goal by using a state-of-the-art perfect crystal based split-and-delay system, capable of splitting individual X-ray pulses and introducing femtosecond to nanosecond time delays. We show the results of an ultrafast hard X-ray photon correlation spectroscopy experiment at LCLS where split X-ray pulses were used to measure the dynamics of gold nanoparticles suspended in hexane. We show how reliable speckle contrast values can be extracted even from verymore » low intensity free electron laser (FEL) speckle patterns by applying maximum likelihood fitting, thus demonstrating the potential of a split-and-delay approach for dynamics measurements at FEL sources. This will enable the characterization of equilibrium and, importantly also reversible non-equilibrium processes in atomically disordered materials.« less

Ultrafast carrier dynamics in GaN/InGaN multiple quantum wells nanorods

NASA Astrophysics Data System (ADS)

Chen, Weijian; Wen, Xiaoming; Latzel, Michael; Yang, Jianfeng; Huang, Shujuan; Shrestha, Santosh; Patterson, Robert; Christiansen, Silke; Conibeer, Gavin

2018-01-01

GaN/InGaN multiple quantum wells (MQW) is a promising material for high-efficiency solid-state lighting. Ultrafast optical pump-probe spectroscopy is an important characterization technique for examining fundamental phenomena in semiconductor nanostructure with sub-picosecond resolution. In this study, ultrafast exciton and charge carrier dynamics in GaN/InGaN MQW planar layer and nanorod are investigated using femtosecond transient absorption (TA) techniques at room temperature. Here nanorods are fabricated by etching the GaN/InGaN MQW planar layers using nanosphere lithography and reactive ion etching. Photoluminescence efficiency of the nanorods have been proved to be much higher than that of the planar layers, but the mechanism of the nanorod structure improvement of PL efficiency is not adequately studied. By comparing the TA profile of the GaN/InGaN MQW planar layers and nanorods, the impact of surface states and nanorods lateral confinement in the ultrafast carrier dynamics of GaN/InGaN MQW is revealed. The nanorod sidewall surface states have a strong influence on the InGaN quantum well carrier dynamics. The ultrafast relaxation processes studied in this GaN/InGaN MQW nanostructure is essential for further optimization of device application.

On the relation between Marcus theory and ultrafast spectroscopy of solvation kinetics

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

Roy, Santanu; Galib, Mirza; Schenter, Gregory K.

The phenomena of solvent exchange control the process of solvating ions, protons, and charged molecules. Building upon our extension of Marcus’ philosophy of electron transfer, here we provide a new perspective of ultrafast solvent exchange mechanism around ions measurable by two-dimensional infrared (2DIR) spectroscopy. In this theory, solvent rearrangement drives an ion-bound water to an activated state of higher coordination number, triggering ion-water separation that leads to the solvent-bound state of the water molecule. This ion-bound to solvent-bound transition rate for a BF 4 --water system is then computed using ab initio molecular dynamics and Marcus theory, and is foundmore » to be in excellent agreement with the 2DIR measurement.« less

On the relation between Marcus theory and ultrafast spectroscopy of solvation kinetics

DOE PAGES

Roy, Santanu; Galib, Mirza; Schenter, Gregory K.; ...

2017-12-24

The phenomena of solvent exchange control the process of solvating ions, protons, and charged molecules. Building upon our extension of Marcus’ philosophy of electron transfer, here we provide a new perspective of ultrafast solvent exchange mechanism around ions measurable by two-dimensional infrared (2DIR) spectroscopy. In this theory, solvent rearrangement drives an ion-bound water to an activated state of higher coordination number, triggering ion-water separation that leads to the solvent-bound state of the water molecule. This ion-bound to solvent-bound transition rate for a BF 4 --water system is then computed using ab initio molecular dynamics and Marcus theory, and is foundmore » to be in excellent agreement with the 2DIR measurement.« less

On the relation between Marcus theory and ultrafast spectroscopy of solvation kinetics

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

Roy, Santanu; Galib, Mirza; Schenter, Gregory K.

The phenomena of solvent exchange control the process of solvating ions, protons, and charged molecules. Building upon our extension of Marcus’ philosophy of electron transfer, we provide a new perspective of ultrafast solvent exchange mechanism around ions measurable by two-dimensional infrared (2DIR) spectroscopy. In this theory, solvent rearrangement drives an ion-bound water to an activated state of higher coordination number, triggering ion-water separation that leads to the solvent-bound state of the water molecule. This ion-bound to solvent-bound transition rate for a BF4- water system is computed using ab initio molecular dynamics and Marcus theory, and is found to be inmore » excellent agreement with the 2DIR measurement.« less

Ultrafast Spectroscopic Noninvasive Probe of Vertical Carrier Transport in Heterostructure Devices (Second year of three year progress report)

DTIC Science & Technology

2014-10-01

properties in Army-relevant semiconductor materials and optoelectronic ( OE ) devices by developing and applying ultrafast optical spectroscopy techniques...met our Q6 through Q8 goals of incorporating electrical testing capabilities into our system, investigating OE devices under operating conditions...extending the capabilities of our system into the IR range, and investigating new OE devices. We have made significant progress towards our Q5 goal of

Serial Femtosecond Crystallography and Ultrafast Absorption Spectroscopy of the Photoswitchable Fluorescent Protein IrisFP.

PubMed

Colletier, Jacques-Philippe; Sliwa, Michel; Gallat, François-Xavier; Sugahara, Michihiro; Guillon, Virginia; Schirò, Giorgio; Coquelle, Nicolas; Woodhouse, Joyce; Roux, Laure; Gotthard, Guillaume; Royant, Antoine; Uriarte, Lucas Martinez; Ruckebusch, Cyril; Joti, Yasumasa; Byrdin, Martin; Mizohata, Eiichi; Nango, Eriko; Tanaka, Tomoyuki; Tono, Kensuke; Yabashi, Makina; Adam, Virgile; Cammarata, Marco; Schlichting, Ilme; Bourgeois, Dominique; Weik, Martin

2016-03-03

Reversibly photoswitchable fluorescent proteins find growing applications in cell biology, yet mechanistic details, in particular on the ultrafast photochemical time scale, remain unknown. We employed time-resolved pump-probe absorption spectroscopy on the reversibly photoswitchable fluorescent protein IrisFP in solution to study photoswitching from the nonfluorescent (off) to the fluorescent (on) state. Evidence is provided for the existence of several intermediate states on the pico- and microsecond time scales that are attributed to chromophore isomerization and proton transfer, respectively. Kinetic modeling favors a sequential mechanism with the existence of two excited state intermediates with lifetimes of 2 and 15 ps, the second of which controls the photoswitching quantum yield. In order to support that IrisFP is suited for time-resolved experiments aiming at a structural characterization of these ps intermediates, we used serial femtosecond crystallography at an X-ray free electron laser and solved the structure of IrisFP in its on state. Sample consumption was minimized by embedding crystals in mineral grease, in which they remain photoswitchable. Our spectroscopic and structural results pave the way for time-resolved serial femtosecond crystallography aiming at characterizing the structure of ultrafast intermediates in reversibly photoswitchable fluorescent proteins.

Gain-guided soliton fiber laser with high-quality rectangle spectrum for ultrafast time-stretch microscopy.

PubMed

Hu, Song; Yao, Jian; Liu, Meng; Luo, Ai-Ping; Luo, Zhi-Chao; Xu, Wen-Cheng

2016-05-16

The ultrafast time-stretch microscopy has been proposed to enhance the temporal resolution of a microscopy system. The optical source is a key component for ultrafast time-stretch microscopy system. Herein, we reported on the gain-guided soliton fiber laser with high-quality rectangle spectrum for ultrafast time-stretch microscopy. By virtue of the excellent characteristics of the gain-guided soliton, the output power and the 3-dB bandwidth of the stable mode-locked soliton could be up to 3 mW and 33.7 nm with a high-quality rectangle shape, respectively. With the proposed robust optical source, the ultrafast time-stretch microscopy with the 49.6 μm resolution and a scan rate of 11 MHz was achieved without the external optical amplification. The obtained results demonstrated that the gain-guided soliton fiber laser could be used as an alternative high-quality optical source for ultrafast time-stretch microscopy and will introduce some applications in fields such as biology, chemical, and optical sensing.

Ultrafast all-optical imaging technique using low-temperature grown GaAs/AlxGa1 - xAs multiple-quantum-well semiconductor

NASA Astrophysics Data System (ADS)

Gao, Guilong; Tian, Jinshou; Wang, Tao; He, Kai; Zhang, Chunmin; Zhang, Jun; Chen, Shaorong; Jia, Hui; Yuan, Fenfang; Liang, Lingliang; Yan, Xin; Li, Shaohui; Wang, Chao; Yin, Fei

2017-11-01

We report and experimentally demonstrate an ultrafast all-optical imaging technique capable of single-shot ultrafast recording with a picosecond-scale temporal resolution and a micron-order two-dimensional spatial resolution. A GaAs/AlxGa1 - xAs multiple-quantum-well (MQW) semiconductor with a picosecond response time, grown using molecular beam epitaxy (MBE) at a low temperature (LT), is used for the first time in ultrafast imaging technology. The semiconductor transforms the signal beam information to the probe beam, the birefringent delay crystal time-serializes the input probe beam, and the beam displacer maps different polarization probe beams onto different detector locations, resulting in two frames with an approximately 9 ps temporal separation and approximately 25 lp/mm spatial resolution in the visible range.

Harmonium: An Ultrafast Vacuum Ultraviolet Facility.

PubMed

Arrell, Christopher A; Ojeda, José; Longetti, Luca; Crepaldi, Alberto; Roth, Silvan; Gatti, Gianmarco; Clark, Andrew; van Mourik, Frank; Drabbels, Marcel; Grioni, Marco; Chergui, Majed

2017-05-31

Harmonium is a vacuum ultraviolet (VUV) photon source built within the Lausanne Centre for Ultrafast Science (LACUS). Utilising high harmonic generation, photons from 20-110 eV are available to conduct steady-state or ultrafast photoelectron and photoion spectroscopies (PES and PIS). A pulse preserving monochromator provides either high energy resolution (70 meV) or high temporal resolution (40 fs). Three endstations have been commissioned for: a) PES of liquids; b) angular resolved PES (ARPES) of solids and; c) coincidence PES and PIS of gas phase molecules or clusters. The source has several key advantages: high repetition rate (up to 15 kHz) and high photon flux (1011 photons per second at 38 eV). The capabilities of the facility complement the Swiss ultrafast and X-ray community (SwissFEL, SLS, NCCR MUST, etc.) helping to maintain Switzerland's leading role in ultrafast science in the world.

Structure and Dynamics with Ultrafast Electron Microscopes

NASA Astrophysics Data System (ADS)

Siwick, Bradley

In this talk I will describe how combining ultrafast lasers and electron microscopes in novel ways makes it possible to directly `watch' the time-evolving structure of condensed matter, both at the level of atomic-scale structural rearrangements in the unit cell and at the level of a material's nano- microstructure. First, I will briefly describe my group's efforts to develop ultrafast electron diffraction using radio- frequency compressed electron pulses in the 100keV range, a system that rivals the capabilities of xray free electron lasers for diffraction experiments. I will give several examples of the new kinds of information that can be gleaned from such experiments. In vanadium dioxide we have mapped the detailed reorganization of the unit cell during the much debated insulator-metal transition. In particular, we have been able to identify and separate lattice structural changes from valence charge density redistribution in the material on the ultrafast timescale. In doing so we uncovered a previously unreported optically accessible phase/state of vanadium dioxide that has monoclinic crystallography like the insulator, but electronic structure and properties that are more like the rutile metal. We have also combined these dynamic structural measurements with broadband ultrafast spectroscopy to make detailed connections between structure and properties for the photoinduced insulator to metal transition. Second, I will show how dynamic transmission electron microscopy (DTEM) can be used to make direct, real space images of nano-microstructural evolution during laser-induced crystallization of amorphous semiconductors at unprecedented spatio-temporal resolution. This is a remarkably complex process that involves several distinct modes of crystal growth and the development of intricate microstructural patterns on the nanosecond to ten microsecond timescales all of which can be imaged directly with DTEM.

Ultrafast Extreme Ultraviolet Spectroscopy of Methylammonium Lead Iodide Perovskite for Carrier Specific Photophysics

NASA Astrophysics Data System (ADS)

Verkamp, Max A.; Lin, Ming-Fu; Ryland, Elizabeth S.; Benke, Kristin; Vura-Weis, Josh

2017-06-01

Methyl ammonium lead iodide (perovskite) is a leading candidate for next-generation solar cell devices. However, the fundamental photophysics responsible for its strong photovoltaic qualities are not fully understood. Ultrafast extreme ultraviolet (XUV) spectroscopy was used to investigate relaxation dynamics in perovskite with carrier specific signals arising from transitions from the common inner-shell level (I 4d) to the valence and conduction bands. Ultrashort (30 fs) pulses of XUV radiation in a broad spectrum (40-70 eV) were obtained using high-harmonic generation in a tabletop instrument. Transient absorption measurements with visible pump and XUV probe directly observed the dynamics of charge carriers after above-band and band-edge excitation.

Ultrafast Spin Crossover in [FeII (bpy)3 ]2+ : Revealing Two Competing Mechanisms by Extreme Ultraviolet Photoemission Spectroscopy.

PubMed

Moguilevski, Alexandre; Wilke, Martin; Grell, Gilbert; Bokarev, Sergey I; Aziz, Saadullah G; Engel, Nicholas; Raheem, Azhr A; Kühn, Oliver; Kiyan, Igor Yu; Aziz, Emad F

2017-03-03

Photoinduced spin-flip in Fe II complexes is an ultrafast phenomenon that has the potential to become an alternative to conventional processing and magnetic storage of information. Following the initial excitation by visible light into the singlet metal-to-ligand charge-transfer state, the electronic transition to the high-spin quintet state may undergo different pathways. Here we apply ultrafast XUV (extreme ultraviolet) photoemission spectroscopy to track the low-to-high spin dynamics in the aqueous iron tris-bipyridine complex, [Fe(bpy) 3 ] 2+ , by monitoring the transient electron density distribution among excited states with femtosecond time resolution. Aided by first-principles calculations, this approach enables us to reveal unambiguously both the sequential and direct de-excitation pathways from singlet to quintet state, with a branching ratio of 4.5:1. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultra-fast all-optical plasmonic switching in near infra-red spectrum using a Kerr nonlinear ring resonator

NASA Astrophysics Data System (ADS)

Nurmohammadi, Tofiq; Abbasian, Karim; Yadipour, Reza

2018-03-01

In this paper, an all-optical plasmonic switch based on metal-insulator-metal (MIM) nanoplasmonic waveguide with a Kerr nonlinear ring resonator is introduced and studied. Two-dimensional simulations utilizing the finite-difference time-domain algorithm are used to demonstrate an apparent optical bistability and significant switching mechanisms (in enabled-low condition: T(ON/OFF) =21.9 and in enabled-high condition: T(ON/OFF) =24.9) of the signal light arisen by altering the pump-light intensity. The proposed all-optical switching demonstrates femtosecond-scale feedback time (90 fs) and then ultra-fast switching can be achieved. The offered all-optical switch may recognize potential significant applications in integrated optical circuits.

Graphene-clad microfibre saturable absorber for ultrafast fibre lasers.

PubMed

Liu, X M; Yang, H R; Cui, Y D; Chen, G W; Yang, Y; Wu, X Q; Yao, X K; Han, D D; Han, X X; Zeng, C; Guo, J; Li, W L; Cheng, G; Tong, L M

2016-05-16

Graphene, whose absorbance is approximately independent of wavelength, allows broadband light-matter interactions with ultrafast responses. The interband optical absorption of graphene can be saturated readily under strong excitation, thereby enabling scientists to exploit the photonic properties of graphene to realize ultrafast lasers. The evanescent field interaction scheme of the propagating light with graphene covered on a D-shaped fibre or microfibre has been employed extensively because of the nonblocking configuration. Obviously, most of the fibre surface is unused in these techniques. Here, we exploit a graphene-clad microfibre (GCM) saturable absorber in a mode-locked fibre laser for the generation of ultrafast pulses. The proposed all-surface technique can guarantee a higher efficiency of light-graphene interactions than the aforementioned techniques. Our GCM-based saturable absorber can generate ultrafast optical pulses within 1.5 μm. This saturable absorber is compatible with current fibre lasers and has many merits such as low saturation intensities, ultrafast recovery times, and wide wavelength ranges. The proposed saturable absorber will pave the way for graphene-based wideband photonics.

Graphene-clad microfibre saturable absorber for ultrafast fibre lasers

PubMed Central

Liu, X. M.; Yang, H. R.; Cui, Y. D.; Chen, G. W.; Yang, Y.; Wu, X. Q.; Yao, X. K.; Han, D. D.; Han, X. X.; Zeng, C.; Guo, J.; Li, W. L.; Cheng, G.; Tong, L. M.

2016-01-01

Graphene, whose absorbance is approximately independent of wavelength, allows broadband light–matter interactions with ultrafast responses. The interband optical absorption of graphene can be saturated readily under strong excitation, thereby enabling scientists to exploit the photonic properties of graphene to realize ultrafast lasers. The evanescent field interaction scheme of the propagating light with graphene covered on a D-shaped fibre or microfibre has been employed extensively because of the nonblocking configuration. Obviously, most of the fibre surface is unused in these techniques. Here, we exploit a graphene-clad microfibre (GCM) saturable absorber in a mode-locked fibre laser for the generation of ultrafast pulses. The proposed all-surface technique can guarantee a higher efficiency of light–graphene interactions than the aforementioned techniques. Our GCM-based saturable absorber can generate ultrafast optical pulses within 1.5 μm. This saturable absorber is compatible with current fibre lasers and has many merits such as low saturation intensities, ultrafast recovery times, and wide wavelength ranges. The proposed saturable absorber will pave the way for graphene-based wideband photonics. PMID:27181419

Photon gating in four-dimensional ultrafast electron microscopy.

PubMed

Hassan, Mohammed T; Liu, Haihua; Baskin, John Spencer; Zewail, Ahmed H

2015-10-20

Ultrafast electron microscopy (UEM) is a pivotal tool for imaging of nanoscale structural dynamics with subparticle resolution on the time scale of atomic motion. Photon-induced near-field electron microscopy (PINEM), a key UEM technique, involves the detection of electrons that have gained energy from a femtosecond optical pulse via photon-electron coupling on nanostructures. PINEM has been applied in various fields of study, from materials science to biological imaging, exploiting the unique spatial, energy, and temporal characteristics of the PINEM electrons gained by interaction with a "single" light pulse. The further potential of photon-gated PINEM electrons in probing ultrafast dynamics of matter and the optical gating of electrons by invoking a "second" optical pulse has previously been proposed and examined theoretically in our group. Here, we experimentally demonstrate this photon-gating technique, and, through diffraction, visualize the phase transition dynamics in vanadium dioxide nanoparticles. With optical gating of PINEM electrons, imaging temporal resolution was improved by a factor of 3 or better, being limited only by the optical pulse widths. This work enables the combination of the high spatial resolution of electron microscopy and the ultrafast temporal response of the optical pulses, which provides a promising approach to attain the resolution of few femtoseconds and attoseconds in UEM.

Photon gating in four-dimensional ultrafast electron microscopy

PubMed Central

Hassan, Mohammed T.; Liu, Haihua; Baskin, John Spencer; Zewail, Ahmed H.

2015-01-01

Ultrafast electron microscopy (UEM) is a pivotal tool for imaging of nanoscale structural dynamics with subparticle resolution on the time scale of atomic motion. Photon-induced near-field electron microscopy (PINEM), a key UEM technique, involves the detection of electrons that have gained energy from a femtosecond optical pulse via photon–electron coupling on nanostructures. PINEM has been applied in various fields of study, from materials science to biological imaging, exploiting the unique spatial, energy, and temporal characteristics of the PINEM electrons gained by interaction with a “single” light pulse. The further potential of photon-gated PINEM electrons in probing ultrafast dynamics of matter and the optical gating of electrons by invoking a “second” optical pulse has previously been proposed and examined theoretically in our group. Here, we experimentally demonstrate this photon-gating technique, and, through diffraction, visualize the phase transition dynamics in vanadium dioxide nanoparticles. With optical gating of PINEM electrons, imaging temporal resolution was improved by a factor of 3 or better, being limited only by the optical pulse widths. This work enables the combination of the high spatial resolution of electron microscopy and the ultrafast temporal response of the optical pulses, which provides a promising approach to attain the resolution of few femtoseconds and attoseconds in UEM. PMID:26438835

Enhanced ultrafast relaxation rate in the Weyl semimetal phase of MoTe2 measured by time- and angle-resolved photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Crepaldi, A.; Autès, G.; Gatti, G.; Roth, S.; Sterzi, A.; Manzoni, G.; Zacchigna, M.; Cacho, C.; Chapman, R. T.; Springate, E.; Seddon, E. A.; Bugnon, Ph.; Magrez, A.; Berger, H.; Vobornik, I.; Kalläne, M.; Quer, A.; Rossnagel, K.; Parmigiani, F.; Yazyev, O. V.; Grioni, M.

2017-12-01

MoTe2 has recently been shown to realize in its low-temperature phase the type-II Weyl semimetal (WSM). We investigated by time- and angle- resolved photoelectron spectroscopy (tr-ARPES) the possible influence of the Weyl points on the electron dynamics above the Fermi level EF, by comparing the ultrafast response of MoTe2 in the trivial and topological phases. In the low-temperature WSM phase, we report an enhanced relaxation rate of electrons optically excited to the conduction band, which we interpret as a fingerprint of the local gap closure when Weyl points form. By contrast, we find that the electron dynamics of the related compound WTe2 is slower and temperature independent, consistent with a topologically trivial nature of this material. Our results shows that tr-ARPES is sensitive to the small modifications of the unoccupied band structure accompanying the structural and topological phase transition of MoTe2.

High-harmonic spectroscopy of ultrafast many-body dynamics in strongly correlated systems

NASA Astrophysics Data System (ADS)

Silva, R. E. F.; Blinov, Igor V.; Rubtsov, Alexey N.; Smirnova, O.; Ivanov, M.

2018-05-01

We bring together two topics that, until now, have been the focus of intense but non-overlapping research efforts. The first concerns high-harmonic generation in solids, which occurs when an intense light field excites a highly non-equilibrium electronic response in a semiconductor or a dielectric. The second concerns many-body dynamics in strongly correlated systems such as the Mott insulator. We show that high-harmonic generation can be used to time-resolve ultrafast many-body dynamics associated with an optically driven phase transition, with accuracy far exceeding one cycle of the driving light field. Our work paves the way for time-resolving highly non-equilibrium many-body dynamics in strongly correlated systems, with few femtosecond accuracy.

Direct Characterization of Ultrafast Energy-Time Entangled Photon Pairs.

PubMed

MacLean, Jean-Philippe W; Donohue, John M; Resch, Kevin J

2018-02-02

Energy-time entangled photons are critical in many quantum optical phenomena and have emerged as important elements in quantum information protocols. Entanglement in this degree of freedom often manifests itself on ultrafast time scales, making it very difficult to detect, whether one employs direct or interferometric techniques, as photon-counting detectors have insufficient time resolution. Here, we implement ultrafast photon counters based on nonlinear interactions and strong femtosecond laser pulses to probe energy-time entanglement in this important regime. Using this technique and single-photon spectrometers, we characterize all the spectral and temporal correlations of two entangled photons with femtosecond resolution. This enables the witnessing of energy-time entanglement using uncertainty relations and the direct observation of nonlocal dispersion cancellation on ultrafast time scales. These techniques are essential to understand and control the energy-time degree of freedom of light for ultrafast quantum optics.

A direct temporal domain approach for ultrafast optical signal processing and its implementation using planar lightwave circuits

NASA Astrophysics Data System (ADS)

Xia, Bing

Ultrafast optical signal processing, which shares the same fundamental principles of electrical signal processing, can realize numerous important functionalities required in both academic research and industry. Due to the extremely fast processing speed, all-optical signal processing and pulse shaping have been widely used in ultrafast telecommunication networks, photonically-assisted RFlmicro-meter waveform generation, microscopy, biophotonics, and studies on transient and nonlinear properties of atoms and molecules. In this thesis, we investigate two types of optical spectrally-periodic (SP) filters that can be fabricated on planar lightwave circuits (PLC) to perform pulse repetition rate multiplication (PRRM) and arbitrary optical waveform generation (AOWG). First, we present a direct temporal domain approach for PRRM using SP filters. We show that the repetition rate of an input pulse train can be multiplied by a factor N using an optical filter with a free spectral range that does not need to be constrained to an integer multiple of N. Furthermore, the amplitude of each individual output pulse can be manipulated separately to form an arbitrary envelope at the output by optimizing the impulse response of the filter. Next, we use lattice-form Mach-Zehnder interferometers (LF-MZI) to implement the temporal domain approach for PRRM. The simulation results show that PRRM with uniform profiles, binary-code profiles and triangular profiles can be achieved. Three silica based LF-MZIs are designed and fabricated, which incorporate multi-mode interference (MMI) couplers and phase shifters. The experimental results show that 40 GHz pulse trains with a uniform envelope pattern, a binary code pattern "1011" and a binary code pattern "1101" are generated from a 10 GHz input pulse train. Finally, we investigate 2D ring resonator arrays (RRA) for ultraf ast optical signal processing. We design 2D RRAs to generate a pair of pulse trains with different binary-code patterns

Electron and lattice dynamics of transition metal thin films observed by ultrafast electron diffraction and transient optical measurements.

PubMed

Nakamura, A; Shimojima, T; Nakano, M; Iwasa, Y; Ishizaka, K

2016-11-01

We report the ultrafast dynamics of electrons and lattice in transition metal thin films (Au, Cu, and Mo) investigated by a combination of ultrafast electron diffraction (UED) and pump-probe optical methods. For a single-crystalline Au thin film, we observe the suppression of the diffraction intensity occuring in 10 ps, which direcly reflects the lattice thermalization via the electron-phonon interaction. By using the two-temperature model, the electron-phonon coupling constant ( g ) and the electron and lattice temperatures ( T e , T l ) are evaluated from UED, with which we simulate the transient optical transmittance. The simulation well agrees with the experimentally obtained transmittance data, except for the slight deviations at the initial photoexcitation and the relaxed quasi-equilibrium state. We also present the results similarly obtained for polycrystalline Au, Cu, and Mo thin films and demonstrate the electron and lattice dynamics occurring in metals with different electron-phonon coupling strengths.

Ultrafast charge separation dynamics in opaque, operational dye-sensitized solar cells revealed by femtosecond diffuse reflectance spectroscopy

PubMed Central

Ghadiri, Elham; Zakeeruddin, Shaik M.; Hagfeldt, Anders; Grätzel, Michael; Moser, Jacques-E.

2016-01-01

Efficient dye-sensitized solar cells are based on highly diffusive mesoscopic layers that render these devices opaque and unsuitable for ultrafast transient absorption spectroscopy measurements in transmission mode. We developed a novel sub-200 femtosecond time-resolved diffuse reflectance spectroscopy scheme combined with potentiostatic control to study various solar cells in fully operational condition. We studied performance optimized devices based on liquid redox electrolytes and opaque TiO2 films, as well as other morphologies, such as TiO2 fibers and nanotubes. Charge injection from the Z907 dye in all TiO2 morphologies was observed to take place in the sub-200 fs time scale. The kinetics of electron-hole back recombination has features in the picosecond to nanosecond time scale. This observation is significantly different from what was reported in the literature where the electron-hole back recombination for transparent films of small particles is generally accepted to occur on a longer time scale of microseconds. The kinetics of the ultrafast electron injection remained unchanged for voltages between +500 mV and –690 mV, where the injection yield eventually drops steeply. The primary charge separation in Y123 organic dye based devices was clearly slower occurring in two picoseconds and no kinetic component on the shorter femtosecond time scale was recorded. PMID:27095505

Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

DOE PAGES

Ma, X.; Fang, F.; Li, Q.; ...

2015-10-28

In this study, optical control of spin is of central importance in the research of ultrafast spintronic devices utilizing spin dynamics at short time scales. Recently developed optical approaches such as ultrafast demagnetization, spin-transfer and spin-orbit torques open new pathways to manipulate spin through its interaction with photon, orbit, charge or phonon. However, these processes are limited by either the long thermal recovery time or the low-temperature requirement. Here we experimentally demonstrate ultrafast coherent spin precession via optical charge-transfer processes in the exchange-coupled Fe/CoO system at room temperature. The efficiency of spin precession excitation is significantly higher and the recoverymore » time of the exchange-coupling torque is much shorter than for the demagnetization procedure, which is desirable for fast switching. The exchange coupling is a key issue in spin valves and tunnelling junctions, and hence our findings will help promote the development of exchange-coupled device concepts for ultrafast coherent spin manipulation.« less

Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

NASA Astrophysics Data System (ADS)

Ma, X.; Fang, F.; Li, Q.; Zhu, J.; Yang, Y.; Wu, Y. Z.; Zhao, H. B.; Lüpke, G.

2015-10-01

Optical control of spin is of central importance in the research of ultrafast spintronic devices utilizing spin dynamics at short time scales. Recently developed optical approaches such as ultrafast demagnetization, spin-transfer and spin-orbit torques open new pathways to manipulate spin through its interaction with photon, orbit, charge or phonon. However, these processes are limited by either the long thermal recovery time or the low-temperature requirement. Here we experimentally demonstrate ultrafast coherent spin precession via optical charge-transfer processes in the exchange-coupled Fe/CoO system at room temperature. The efficiency of spin precession excitation is significantly higher and the recovery time of the exchange-coupling torque is much shorter than for the demagnetization procedure, which is desirable for fast switching. The exchange coupling is a key issue in spin valves and tunnelling junctions, and hence our findings will help promote the development of exchange-coupled device concepts for ultrafast coherent spin manipulation.

Single-order laser high harmonics in XUV for ultrafast photoelectron spectroscopy of molecular wavepacket dynamics.

PubMed

Fushitani, Mizuho; Hishikawa, Akiyoshi

2016-11-01

We present applications of extreme ultraviolet (XUV) single-order laser harmonics to gas-phase ultrafast photoelectron spectroscopy. Ultrashort XUV pulses at 80 nm are obtained as the 5th order harmonics of the fundamental laser at 400 nm by using Xe or Kr as the nonlinear medium and separated from other harmonic orders by using an indium foil. The single-order laser harmonics is applied for real-time probing of vibrational wavepacket dynamics of I 2 molecules in the bound and dissociating low-lying electronic states and electronic-vibrational wavepacket dynamics of highly excited Rydberg N 2 molecules.

Electrically-driven GHz range ultrafast graphene light emitter (Conference Presentation)

NASA Astrophysics Data System (ADS)

Kim, Youngduck; Gao, Yuanda; Shiue, Ren-Jye; Wang, Lei; Aslan, Ozgur Burak; Kim, Hyungsik; Nemilentsau, Andrei M.; Low, Tony; Taniguchi, Takashi; Watanabe, Kenji; Bae, Myung-Ho; Heinz, Tony F.; Englund, Dirk R.; Hone, James

2017-02-01

Ultrafast electrically driven light emitter is a critical component in the development of the high bandwidth free-space and on-chip optical communications. Traditional semiconductor based light sources for integration to photonic platform have therefore been heavily studied over the past decades. However, there are still challenges such as absence of monolithic on-chip light sources with high bandwidth density, large-scale integration, low-cost, small foot print, and complementary metal-oxide-semiconductor (CMOS) technology compatibility. Here, we demonstrate the first electrically driven ultrafast graphene light emitter that operate up to 10 GHz bandwidth and broadband range (400 1600 nm), which are possible due to the strong coupling of charge carriers in graphene and surface optical phonons in hBN allow the ultrafast energy and heat transfer. In addition, incorporation of atomically thin hexagonal boron nitride (hBN) encapsulation layers enable the stable and practical high performance even under the ambient condition. Therefore, electrically driven ultrafast graphene light emitters paves the way towards the realization of ultrahigh bandwidth density photonic integrated circuits and efficient optical communications networks.

Broadband ultrafast nonlinear absorption and nonlinear refraction of layered molybdenum dichalcogenide semiconductors

NASA Astrophysics Data System (ADS)

Wang, Kangpeng; Feng, Yanyan; Chang, Chunxia; Zhan, Jingxin; Wang, Chengwei; Zhao, Quanzhong; Coleman, Jonathan N.; Zhang, Long; Blau, Werner J.; Wang, Jun

2014-08-01

A series of layered molybdenum dichalcogenides, i.e., MoX2 (X = S, Se and Te), were prepared in cyclohexyl pyrrolidinone by a liquid-phase exfoliation technique. The high quality of the two-dimensional nanostructures was verified by transmission electron microscopy and absorption spectroscopy. Open- and closed-aperture Z-scans were employed to study the nonlinear absorption and nonlinear refraction of the MoX2 dispersions, respectively. All the three-layered nanostructures exhibit prominent ultrafast saturable absorption (SA) for both femtosecond (fs) and picosecond (ps) laser pulses over a broad wavelength range from the visible to the near infrared. While the dispersions treated with low-speed centrifugation (1500 rpm) have an SA response, and the MoS2 and MoSe2 dispersions after higher speed centrifugation (10 000 rpm) possess two-photon absorption for fs pulses at 1030 nm, which is due to the significant reduction of the average thickness of the nanosheets; hence, the broadening of band gap. In addition, all dispersions show obvious nonlinear self-defocusing for ps pulses at both 1064 nm and 532 nm, resulting from the thermally-induced nonlinear refractive index. The versatile ultrafast nonlinear properties imply a huge potential of the layered MoX2 semiconductors in the development of nanophotonic devices, such as mode-lockers, optical limiters, optical switches, etc.A series of layered molybdenum dichalcogenides, i.e., MoX2 (X = S, Se and Te), were prepared in cyclohexyl pyrrolidinone by a liquid-phase exfoliation technique. The high quality of the two-dimensional nanostructures was verified by transmission electron microscopy and absorption spectroscopy. Open- and closed-aperture Z-scans were employed to study the nonlinear absorption and nonlinear refraction of the MoX2 dispersions, respectively. All the three-layered nanostructures exhibit prominent ultrafast saturable absorption (SA) for both femtosecond (fs) and picosecond (ps) laser pulses over a broad

Ultrafast atomic-scale visualization of acoustic phonons generated by optically excited quantum dots

PubMed Central

Vanacore, Giovanni M.; Hu, Jianbo; Liang, Wenxi; Bietti, Sergio; Sanguinetti, Stefano; Carbone, Fabrizio; Zewail, Ahmed H.

2017-01-01

Understanding the dynamics of atomic vibrations confined in quasi-zero dimensional systems is crucial from both a fundamental point-of-view and a technological perspective. Using ultrafast electron diffraction, we monitored the lattice dynamics of GaAs quantum dots—grown by Droplet Epitaxy on AlGaAs—with sub-picosecond and sub-picometer resolutions. An ultrafast laser pulse nearly resonantly excites a confined exciton, which efficiently couples to high-energy acoustic phonons through the deformation potential mechanism. The transient behavior of the measured diffraction pattern reveals the nonequilibrium phonon dynamics both within the dots and in the region surrounding them. The experimental results are interpreted within the theoretical framework of a non-Markovian decoherence, according to which the optical excitation creates a localized polaron within the dot and a travelling phonon wavepacket that leaves the dot at the speed of sound. These findings indicate that integration of a phononic emitter in opto-electronic devices based on quantum dots for controlled communication processes can be fundamentally feasible. PMID:28852685

Elucidating the Structure of Sugars: MW Spectroscopy Combined with Ultrafast UV Laser Vaporization

NASA Astrophysics Data System (ADS)

Cocinero, Emilio J.; Ecija, Patricia; Basterretxea, Francisco J.; Fernandez, Jose A.; Castano, Fernando; Lesarri, Alberto; Grabow, Jens-Uwe; Cimas, Alvaro

2013-06-01

Carbohydrates are one of the most versatile biochemicalbuilding blocks, widely acting in energetic, structural or recognition processes. Even the small monosaccharides display unique structural and conformational freedom and may coexist in many open-chain or cyclic forms. We recently initiated the investigation of a series of monosaccharides using a combination of ultrafast laser vaporization and microwave spectroscopy in supersonic jet expansions. We present several structural studies on carbohydrates of aldoses and ketoses of five and six carbon sugars vaporized by UV ultrafast laser vaporization and stabilized in a jet expansion. The experimental evidence confirms that sugars exhibits a α-/β-pyranose conformation (6-membered ring), sharply contrasting with the furanose form (5-membered ring) found in the nature (as component of RNA, sucrose). In addition, thanks to the use of enriched samples, we have experimentally determined the substitution and effective structures. Finally, the structure of several monosaccharides was compared and common structural patterns of their conformational landscape will be showed. E. J. Cocinero, A. Lesarri, P. écija, F. J. Basterretxea, J. U. Grabow, J. A. Fernández and F. Castaño Angew. Chem. Int. Ed. 51, 3119-3124, 2012. E. J. Cocinero, A. Lesarri, P. écija, Á. Cimas, B. G. Davis, F. J. Basterretxea, J. A. Fernández and F. Castaño J. Am. Chem. Soc. 135, 2845-2852, 2013.

Ultrafast Spectral Diffusion of the First Subband Exciton in Single-Wall Carbon Nanotubes

NASA Astrophysics Data System (ADS)

Schilling, Daniel; Hertel, Tobias

2013-03-01

The width of optical transitions in semiconductors is determined by homogeneous and inhomogeneous contributions. Here, we report on the determination of homogeneous linewidths for the first exciton subband transition and the dynamics of spectral diffusion in single-wall carbon nanotubes (SWNTs) using one- and two-dimensional time resolved spectral hole burning spectroscopy. Our investigation of highly purified semiconducting (6,5)-SWNTs suggests that room temperature homogeneous linewidths are on the order of 4 meV and are rapidly broadened by an ultrafast sub-ps spectral diffusion process. These findings are supported by our off-resonant excitation experiments where we observe sub-ps population transfer reflecting the thermal distribution of energy levels around the first subband exciton transition. The results of temperature-dependent spectral hole burning experiments between 17 K and 293 K suggest that homogeneous linewidths are due to exciton interaction with low energy optical phonons, most likely of the radial breathing mode type. In contrast, we find that inhomogeneous broadening is determined by an electronic degree of freedom such as ultrafast intra-tube exciton diffusion which is characteristic and unique for excitons in these one-dimensional semiconductors.

Ultrafast dynamics and stabilization in chip-scale optical frequency combs (Conference Presentation)

NASA Astrophysics Data System (ADS)

Huang, Shu Wei

2017-02-01

Optical frequency comb technology has been the cornerstone for scientific breakthroughs such as precision frequency metrology, re-definition of time, extreme light-matter interaction, and attosecond sciences. Recently emerged Kerr-active microresonators are promising alternatives to the current benchmark femtosecond laser platform. These chip-scale frequency combs, or Kerr combs, are unique in their compact footprints and offer the potential for monolithic electronic and feedback integration, thereby expanding the already remarkable applications of optical frequency combs. In this talk, I will first report the generation and characterization of low-phase-noise Kerr frequency combs. Measurements of the Kerr comb ultrafast dynamics and phase noise will be presented and discussed. Then I will describe novel strategies to fully stabilize Kerr comb line frequencies towards chip-scale optical frequency synthesizers with a relative uncertainty better than 2.7×10-16. I will show that the unique generation physics of Kerr frequency comb can provide an intrinsic self-referenced access to the Kerr comb line frequencies. The strategy improves the optical frequency stability by more than two orders of magnitude, while preserving the Kerr comb's key advantage of low SWaP and potential for chip-scale electronic and photonic integration.

Ultrafast nonlinear optical properties of thin-solid DNA film and their application as a saturable absorber in femtosecond mode-locked fiber laser

PubMed Central

Khazaeinezhad, Reza; Hosseinzadeh Kassani, Sahar; Paulson, Bjorn; Jeong, Hwanseong; Gwak, Jiyoon; Rotermund, Fabian; Yeom, Dong-Il; Oh, Kyunghwan

2017-01-01

A new extraordinary application of deoxyribonucleic acid (DNA) thin-solid-film was experimentally explored in the field of ultrafast nonlinear photonics. Optical transmission was investigated in both linear and nonlinear regimes for two types of DNA thin-solid-films made from DNA in aqueous solution and DNA-cetyltrimethylammonium chloride (CTMA) in an organic solvent. Z-scan measurements revealed a high third-order nonlinearity with n2 exceeding 10−9 at a wavelength of 1570 nm, for a nonlinarity about five orders of magnitude larger than that of silica. We also demonstrated ultrafast saturable absorption (SA) with a modulation depth of 0.43%. DNA thin solid films were successfully deposited on a side-polished optical fiber, providing an efficient evanescent wave interaction. We built an organic-inorganic hybrid all-fiber ring laser using DNA film as an ultrafast SA and using Erbium-doped fiber as an efficient optical gain medium. Stable transform-limited femtosecond soliton pulses were generated with full width half maxima of 417 fs for DNA and 323 fs for DNA-CTMA thin-solid-film SAs. The average output power was 4.20 mW for DNA and 5.46 mW for DNA-CTMA. Detailed conditions for DNA solid film preparation, dispersion control in the laser cavity and subsequent characteristics of soliton pulses are discussed, to confirm unique nonlinear optical applications of DNA thin-solid-film. PMID:28128340

Development of a high brightness ultrafast Transmission Electron Microscope based on a laser-driven cold field emission source.

PubMed

Houdellier, F; Caruso, G M; Weber, S; Kociak, M; Arbouet, A

2018-03-01

We report on the development of an ultrafast Transmission Electron Microscope based on a cold field emission source which can operate in either DC or ultrafast mode. Electron emission from a tungsten nanotip is triggered by femtosecond laser pulses which are tightly focused by optical components integrated inside a cold field emission source close to the cathode. The properties of the electron probe (brightness, angular current density, stability) are quantitatively determined. The measured brightness is the largest reported so far for UTEMs. Examples of imaging, diffraction and spectroscopy using ultrashort electron pulses are given. Finally, the potential of this instrument is illustrated by performing electron holography in the off-axis configuration using ultrashort electron pulses. Copyright © 2017 Elsevier B.V. All rights reserved.

Femtosecond Optical and X-Ray Measurement of the Semiconductor-to-Metal Transition in VO2

NASA Astrophysics Data System (ADS)

Cavalleri, Andrea; Toth, Csaba; Squier, Jeff; Siders, Craig; Raksi, Ferenc; Forget, Patrick; Kieffer, Jean-Claude

2001-03-01

While the use of ultrashort visible pulses allows access to ultrafast changes in the optical properties during phase transitions, measurement of the correlation between atomic movement and electronic rearrangement has proven more elusive. Here, we report on the conjunct measurement of ultrafast electronic and structural dynamics during a semiconductor-to-metal phase transition in VO2. Rearrangement of the unit cell from monoclinic to rutile (measured by ultrafast x-ray diffraction) is accompanied by a sharp increase in the electrical conductivity and perturbation of the optical properties (measured with ultrafast visible spectroscopy). Ultrafast x-ray diffraction experiments were performed using femtosecond bursts of Cu-Ka from a laser generated plasma source. A clear rise of the diffraction signal originating from the impulsively generated metallic phase was observable on the sub-picosecond timescale. Optical experiments were performed using time-resolved microscopy, providing temporally and spatially resolved measurements of the optical reflectivity at 800 nm. The data indicate that the reflectivity of the low-temperature semiconducting solid is driven to that of the equilibrium, high-temperature metallic phase within 400 fs after irradiation with a 50-fs laser pulse at fluences in excess of 10 mJ/cm2. In conclusion, the data presented in this contribution suggest that the semiconductor-to-metal transition in VO2 occurs within 500 fs after laser-irradiation. A nonthermal physical mechanism governs the re-arrangement.

Towards simultaneous measurements of electronic and structural properties in ultra-fast x-ray free electron laser absorption spectroscopy experiments

NASA Astrophysics Data System (ADS)

Gaudin, J.; Fourment, C.; Cho, B. I.; Engelhorn, K.; Galtier, E.; Harmand, M.; Leguay, P. M.; Lee, H. J.; Nagler, B.; Nakatsutsumi, M.; Ozkan, C.; Störmer, M.; Toleikis, S.; Tschentscher, Th; Heimann, P. A.; Dorchies, F.

2014-04-01

The rapidly growing ultrafast science with X-ray lasers unveils atomic scale processes with unprecedented time resolution bringing the so called ``molecular movie'' within reach. X-ray absorption spectroscopy is one of the most powerful x-ray techniques providing both local atomic order and electronic structure when coupled with ad-hoc theory. Collecting absorption spectra within few x-ray pulses is possible only in a dispersive setup. We demonstrate ultrafast time-resolved measurements of the LIII-edge x-ray absorption near-edge spectra of irreversibly laser excited Molybdenum using an average of only few x-ray pulses with a signal to noise ratio limited only by the saturation level of the detector. The simplicity of the experimental set-up makes this technique versatile and applicable for a wide range of pump-probe experiments, particularly in the case of non-reversible processes.

3D microstructuring inside glass by ultrafast laser

NASA Astrophysics Data System (ADS)

Sugioka, Koji; Hanada, Yasutaka; Midorikawa, Katsumi; Kawano, Hiroyuki; Ishikawa, Ikuko S.; Miyawaki, Atsushi

2012-01-01

We demonstrate three-dimensional (3D) microstructuring inside glass by ultrafast laser to fabricate microfluidic chips integrated with some functional microcomponents such as optical attenuators and optical waveguides. The fabricated microchips are applied to understand phenomena and functions of microorganisms and cyanobacteria. Ultrafast laser irradiation followed by thermal treatment and wet etching in dilute hydrofluoric acid solution resulted in fabrication of 3D microfludic structures embedded in a photosensitive glass. The embedded microfludic structures enabled us to easily and efficiently observe Phormidium gliding to the seedling root, which accelerates growth of the vegetable. In addition, integration of optical attenuators and optical waveguides into the microfluidic structures clarified the mechanism of the gliding movement of Phormidium. We termed such integrated microchips nanoaquariums, realizing the highly efficient and functional observation and analysis of various microorganisms.

Applications of telecommunication technology for optical instrumentation with an emphasis on space-time duality

NASA Astrophysics Data System (ADS)

van Howe, James William

Telecommunication technology has often been applied to areas of science and engineering seemingly unrelated to communication systems. Innovations such as electronic amplifiers, the transistor, digital coding, optical fiber, and the laser, which all had roots in communication technology, have been implemented in devices from bar-code scanners to fiber endoscopes for medical procedures. In the same way, the central theme of the work in the following chapters has been to borrow both the concepts and technology of telecommunications systems to develop novel optical instrumentation for non-telecom pursuits. This work particularly leverages fiber-integrated electro-optic phase modulators to apply custom phase profiles to ultrafast pulses for control and manipulation. Such devices are typically used in telecom transmitters to encode phase data onto optical pulses (differential phase-shift keying), or for chirped data transmission. We, however, use electro-optic phase modulators to construct four novel optical devices: (1) a programmable ultrafast optical delay line with record scanning speed for applications in optical metrology, interferometry, or broad-band phase arrays, (2) a multiwavelength pulse generator for real-time optical sampling of electronic waveforms, (3) a simple femtosecond pulse generator for uses in biomedical imaging or ultrafast spectroscopy, and (4) a nonlinear phase compensator to increase the energy of fiber-amplified ultrashort pulse systems. In addition, we describe a fifth instrument which makes use of a higher-order mode fiber, similar in design to dispersion compensating fibers used for telecom. Through soliton self-frequency shift in the higher-order mode fiber, we can broadly-tune the center frequency of ultrashort pulses in energy regimes useful for biomedical imaging or ultrafast spectroscopy. The advantages gained through using telecom components in each of these systems are the simplicity and robustness of all-fiber configurations, high

A highly ordered mesostructured material containing regularly distributed phenols: preparation and characterization at a molecular level through ultra-fast magic angle spinning proton NMR spectroscopy.

PubMed

Roussey, Arthur; Gajan, David; Maishal, Tarun K; Mukerjee, Anhurada; Veyre, Laurent; Lesage, Anne; Emsley, Lyndon; Copéret, Christophe; Thieuleux, Chloé

2011-03-14

Highly ordered organic-inorganic mesostructured material containing regularly distributed phenols is synthesized by combining a direct synthesis of the functional material and a protection-deprotection strategy and characterized at a molecular level through ultra-fast magic angle spinning proton NMR spectroscopy.

Ultrafast electron-lattice coupling dynamics in VO2 and V2O3 thin films

NASA Astrophysics Data System (ADS)

Abreu, Elsa; Gilbert Corder, Stephanie N.; Yun, Sun Jin; Wang, Siming; Ramírez, Juan Gabriel; West, Kevin; Zhang, Jingdi; Kittiwatanakul, Salinporn; Schuller, Ivan K.; Lu, Jiwei; Wolf, Stuart A.; Kim, Hyun-Tak; Liu, Mengkun; Averitt, Richard D.

2017-09-01

Ultrafast optical pump-optical probe and optical pump-terahertz probe spectroscopy were performed on vanadium dioxide (VO2) and vanadium sesquioxide (V2O3 ) thin films over a wide temperature range. A comparison of the experimental data from these two different techniques and two different vanadium oxides, in particular a comparison of the spectral weight oscillations generated by the photoinduced longitudinal acoustic modulation, reveals the strong electron-phonon coupling that exists in both materials. The low-energy Drude response of V2O3 appears more amenable than VO2 to ultrafast strain control. Additionally, our results provide a measurement of the temperature dependence of the sound velocity in both systems, revealing a four- to fivefold increase in VO2 and a three- to fivefold increase in V2O3 across the insulator-to-metal phase transition. Our data also confirm observations of strong damping and phonon anharmonicity in the metallic phase of VO2, and suggest that a similar phenomenon might be at play in the metallic phase of V2O3 . More generally, our simple table-top approach provides relevant and detailed information about dynamical lattice properties of vanadium oxides, paving the way to similar studies in other complex materials.

Ultrafast optical measurements of surface waves on a patterned layered nanostructure

NASA Astrophysics Data System (ADS)

Daly, Brian; Bjornsson, Matteo; Connolly, Aine; Mahat, Sushant; Rachmilowitz, Bryan; Antonelli, George; Myers, Alan; Yoo, Hui-Jae; Singh, Kanwal; King, Sean

2015-03-01

We report ultrafast optical pump-probe measurements of 12 - 54 GHz surface acoustic waves (SAWs) on patterned layered nanostructures. These very high frequency SAWs were generated and detected on the following patterned film stack: 25 nm physically vapor deposited TiN / 180 nm porous PECVD-grown a-SiOC:H dielectric / 12 nm non-porous PECVD-grown a-SiOC:H etch-stop / 100 nm CVD-grown a-SiO2 / Si (100) substrate. The TiN layer was dry plasma etched to form lines of rectangular cross section with pitches of 420 nm, 250 nm, 180 nm, and 168 nm and the lines were oriented parallel to the [110] direction on the wafer surface. The absorption of ultrafast pulses from a Ti:sapphire oscillator operating at 800 nm generated SAWs that were detected by time-delayed probe pulses from the same oscillator via a reflectivity change (ΔR) . In each of the four cases the SAW frequency increased with decreasing pitch, but not in a linear way as had been seen in previous experiments of this sort. By comparing the results with mechanical simulations, we present evidence for the detection of different types of SAWs in each case, including Rayleigh-like waves, Sezawa waves, and leaky or radiative waves. This work was supported by NSF Award DMR1206681.

Intermolecular dynamics of substitued benzene and cyclohexane liquids, studied by femtosecond nonlinear-optical polarization spectroscopy

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

Chang, Y.J.; Castner, E.W. Jr.

Femtosecond time-resolved optical-heterodyne detected Raman-induced Kerr effect spectroscopy (OHD-RIKES) is shown to be a powerful and comprehensive tool for studying the intermolecular dynamics occurring in liquids. The observed dynamics include both the underdamped or coherent inertial motions, and the longer time scale diffusive relaxation. The inertial dynamics include phonon-like intermolecular vibrations, intermolecular collisions, and librational caging motions. Data are presented and analyzed for a series of five liquids: cyclohexane, methylcyclohexane, toluene, benzyl alcohol, and benzonitrile, listed in order of increasing polarity. We explore the effects of aromaticity (e.g., methylcyclohexane vs toluene), symmetry reduction (cyclohexane vs methylcyclohexane), and substitution effects (e.g.,more » substituted benzene series) on the ultrafast intermolecular dynamics, for a group of molecular liquids of similar size and volume. We analyze the intermolecular dynamics in both the time and frequency domains by means of Fourier transformations. When Fourier-transformed into the frequency domain, the OHD-RIKES ultrafast transients of the intermolecular dynamics can be directly compared with the frequency domain spectra obtained from the far-infrared absorption and depolarized Raman techniques. This is done using the Gaussian librational caging model of Lynden-Bell and Steele, which results in a power-law scaling relation between dipole and polarizability time correlation functions. 122 refs., 7 figs., 7 tabs.« less

Broadband ultrafast nonlinear absorption and nonlinear refraction of layered molybdenum dichalcogenide semiconductors.

PubMed

Wang, Kangpeng; Feng, Yanyan; Chang, Chunxia; Zhan, Jingxin; Wang, Chengwei; Zhao, Quanzhong; Coleman, Jonathan N; Zhang, Long; Blau, Werner J; Wang, Jun

2014-09-21

A series of layered molybdenum dichalcogenides, i.e., MoX₂ (X = S, Se and Te), were prepared in cyclohexyl pyrrolidinone by a liquid-phase exfoliation technique. The high quality of the two-dimensional nanostructures was verified by transmission electron microscopy and absorption spectroscopy. Open- and closed-aperture Z-scans were employed to study the nonlinear absorption and nonlinear refraction of the MoX₂ dispersions, respectively. All the three-layered nanostructures exhibit prominent ultrafast saturable absorption (SA) for both femtosecond (fs) and picosecond (ps) laser pulses over a broad wavelength range from the visible to the near infrared. While the dispersions treated with low-speed centrifugation (1500 rpm) have an SA response, and the MoS₂ and MoSe₂ dispersions after higher speed centrifugation (10,000 rpm) possess two-photon absorption for fs pulses at 1030 nm, which is due to the significant reduction of the average thickness of the nanosheets; hence, the broadening of band gap. In addition, all dispersions show obvious nonlinear self-defocusing for ps pulses at both 1064 nm and 532 nm, resulting from the thermally-induced nonlinear refractive index. The versatile ultrafast nonlinear properties imply a huge potential of the layered MoX2 semiconductors in the development of nanophotonic devices, such as mode-lockers, optical limiters, optical switches, etc.

Femtosecond timing measurement and control using ultrafast organic thin films

NASA Astrophysics Data System (ADS)

Naruse, Makoto; Mitsu, Hiroyuki; Furuki, Makoto; Iwasa, Izumi; Sato, Yasuhiro; Tatsuura, Satoshi; Tian, Minquan

2003-12-01

We show a femtosecond timing measurement and control technique using a squarylium dye J-aggregate film, which is an organic thin film that acts as an ultrafast two-dimensional optical switch. Optical pulse timing is directly mapped to space-domain position on the film, and the large area and ultrafast response offer a femtosecond-resolved, large dynamic range, real-time, multichannel timing measurement capability. A timing fluctuation (jitter, wander, and skew) reduction architecture is presented and experimentally demonstrated.

Ultrafast Optical Modulation of Second- and Third-Harmonic Generation from Cut-Disk-Based Metasurfaces

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

Sartorello, Giovanni; Olivier, Nicolas; Zhang, Jingjing

2016-08-17

We design and fabricate a metasurface composed of gold cut-disk resonators that exhibits a strong coherent nonlinear response. We experimentally demonstrate all-optical modulation of both second- and third-harmonic signals on a subpicosecond time scale. Pump probe experiments and numerical models show that the observed effects are due to the ultrafast response of the electronic excitations in the metal under external illumination. These effects pave the way for the development of novel active nonlinear metasurfaces with controllable and switchable coherent nonlinear response.

Towards simultaneous measurements of electronic and structural properties in ultra-fast x-ray free electron laser absorption spectroscopy experiments

PubMed Central

Gaudin, J.; Fourment, C.; Cho, B. I.; Engelhorn, K.; Galtier, E.; Harmand, M.; Leguay, P. M.; Lee, H. J.; Nagler, B.; Nakatsutsumi, M.; Ozkan, C.; Störmer, M.; Toleikis, S.; Tschentscher, Th; Heimann, P. A.; Dorchies, F.

2014-01-01

The rapidly growing ultrafast science with X-ray lasers unveils atomic scale processes with unprecedented time resolution bringing the so called “molecular movie” within reach. X-ray absorption spectroscopy is one of the most powerful x-ray techniques providing both local atomic order and electronic structure when coupled with ad-hoc theory. Collecting absorption spectra within few x-ray pulses is possible only in a dispersive setup. We demonstrate ultrafast time-resolved measurements of the LIII-edge x-ray absorption near-edge spectra of irreversibly laser excited Molybdenum using an average of only few x-ray pulses with a signal to noise ratio limited only by the saturation level of the detector. The simplicity of the experimental set-up makes this technique versatile and applicable for a wide range of pump-probe experiments, particularly in the case of non-reversible processes. PMID:24740172

Towards simultaneous measurements of electronic and structural properties in ultra-fast x-ray free electron laser absorption spectroscopy experiments

DOE PAGES

Gaudin, J.; Fourment, C.; Cho, B. I.; ...

2014-04-17

The rapidly growing ultrafast science with X-ray lasers unveils atomic scale processes with unprecedented time resolution bringing the so called “molecular movie” within reach. X-ray absorption spectroscopy is one of the most powerful x-ray techniques providing both local atomic order and electronic structure when coupled with ad-hoc theory. Collecting absorption spectra within few x-ray pulses is possible only in a dispersive setup. We demonstrate ultrafast time-resolved measurements of the LIII-edge x-ray absorption near-edge spectra of irreversibly laser excited Molybdenum using an average of only few x-ray pulses with a signal to noise ratio limited only by the saturation level ofmore » the detector. The simplicity of the experimental set-up makes this technique versatile and applicable for a wide range of pump-probe experiments, particularly in the case of non-reversible processes.« less

Low-threshold ultrafast all-optical switch implemented with metallic nanoshells in the photonic crystal ring resonator

NASA Astrophysics Data System (ADS)

Ghadrdan, Majid; Mansouri-Birjandi, Mohammad Ali

2017-11-01

An all-optical switch based on nonlinear photonic crystal ring resonator embedded with silica dielectric surrounded by silver nanoshell (NS) inside the ring resonator has been introduced and analyzed in this article. We considered silica with radius of 10 nm and silver with radius of 16 nm as core and shell, respectively. By placing NSs inside the photonic crystal ring resonator, we succeeded in reducing the threshold power to 12.8 mW/μm2 and the switching time to about 0.4 ps. The results of this research suggest a new technique for reducing switching light intensity. With small size, ultra-fast switching time, and low-threshold power, the structure has the potential to be applied in optical integration circuits and nanoscale optical chips.

Ultrafast dynamics during the photoinduced phase transition in VO2

NASA Astrophysics Data System (ADS)

Wegkamp, Daniel; Stähler, Julia

2015-12-01

The phase transition of VO2 from a monoclinic insulator to a rutile metal, which occurs thermally at TC = 340 K, can also be driven by strong photoexcitation. The ultrafast dynamics during this photoinduced phase transition (PIPT) have attracted great scientific attention for decades, as this approach promises to answer the question of whether the insulator-to-metal (IMT) transition is caused by electronic or crystallographic processes through disentanglement of the different contributions in the time domain. We review our recent results achieved by femtosecond time-resolved photoelectron, optical, and coherent phonon spectroscopy and discuss them within the framework of a selection of latest, complementary studies of the ultrafast PIPT in VO2. We show that the population change of electrons and holes caused by photoexcitation launches a highly non-equilibrium plasma phase characterized by enhanced screening due to quasi-free carriers and followed by two branches of non-equilibrium dynamics: (i) an instantaneous (within the time resolution) collapse of the insulating gap that precedes charge carrier relaxation and significant ionic motion and (ii) an instantaneous lattice potential symmetry change that represents the onset of the crystallographic phase transition through ionic motion on longer timescales. We discuss the interconnection between these two non-thermal pathways with particular focus on the meaning of the critical fluence of the PIPT in different types of experiments. Based on this, we conclude that the PIPT threshold identified in optical experiments is most probably determined by the excitation density required to drive the lattice potential change rather than the IMT. These considerations suggest that the IMT can be driven by weaker excitation, predicting a transiently metallic, monoclinic state of VO2 that is not stabilized by the non-thermal structural transition and, thus, decays on ultrafast timescales.

Shock waves in molecular solids: ultrafast vibrational spectroscopy of the first nanosecond

NASA Astrophysics Data System (ADS)

Franken, J.; Hambir, S. A.; Hare, D. E.; Dlott, D. D.

A novel technique which uses a microfabricated shock target array assembly is described, where the passage of a shock front through a thin (0.5μm) polycrystalline layer and the subsequent unloading process is monitored in real time with ultrafast coherent Raman spectroscopy. Using a high repetition rate laser shock generation technique, high resolution, coherent Raman spectra are obtained in shocked anthracene and in a high explosive material, NTO, with time resolution of 50 ps. Spectroscopic measurements are presented which yield the shock pressure (up to 5 GPa), the shock velocity ( 4 km/s), the shock front risetime (tr < 25 ps), and the temperature ( 400°C). A brief discussion is presented, how this new technique can be used to determine the Hugoniot, the equation of state, the entropy increase across the shock front, and monitor shock induced chemical reactions in real time.

Review of optical breast imaging and spectroscopy

NASA Astrophysics Data System (ADS)

Grosenick, Dirk; Rinneberg, Herbert; Cubeddu, Rinaldo; Taroni, Paola

2016-09-01

Diffuse optical imaging and spectroscopy of the female breast is an area of active research. We review the present status of this field and discuss the broad range of methodologies and applications. Starting with a brief overview on breast physiology, the remodeling of vasculature and extracellular matrix caused by solid tumors is highlighted that is relevant for contrast in optical imaging. Then, the various instrumental techniques and the related methods of data analysis and image generation are described and compared including multimodality instrumentation, fluorescence mammography, broadband spectroscopy, and diffuse correlation spectroscopy. We review the clinical results on functional properties of malignant and benign breast lesions compared to host tissue and discuss the various methods to improve contrast between healthy and diseased tissue, such as enhanced spectroscopic information, dynamic variations of functional properties, pharmacokinetics of extrinsic contrast agents, including the enhanced permeability and retention effect. We discuss research on monitoring neoadjuvant chemotherapy and on breast cancer risk assessment as potential clinical applications of optical breast imaging and spectroscopy. Moreover, we consider new experimental approaches, such as photoacoustic imaging and long-wavelength tissue spectroscopy.

The complete optical oscilloscope

NASA Astrophysics Data System (ADS)

Lei, Cheng; Goda, Keisuke

2018-04-01

Observing ultrafast transient dynamics in optics is a challenging task. Two teams in Europe have now independently developed `optical oscilloscopes' that can capture both amplitude and phase information of ultrafast optical signals. Their schemes yield new insights into the nonlinear physics that takes place inside optical fibres.

Ultrafast Unzipping of a Beta-Hairpin Peptide

NASA Astrophysics Data System (ADS)

Zinth, W.; Schrader, T. E.; Schreier, W. J.; Koller, F. O.; Cordes, T.; Babitzki, G.; Denschlag, R.; Tavan, P.; Löweneck, M.; Dong, Shou-Liang; Moroder, L.; Renner, C.

Light induced switching of a beta-hairpin structure is investigated by femtosecond IR spectroscopy. While the unzipping process comprises ultrafast kinetics and is finished within 1 ns, the folding into the hairpin structure is a much slower process.

650-nJ pulses from a cavity-dumped Yb:fiber-pumped ultrafast optical parametric oscillator

NASA Astrophysics Data System (ADS)

Lamour, Tobias P.; Reid, Derryck T.

2011-08-01

Sub-250-fs pulses with energies of up to 650 nJ and peak powers up to 2.07 MW were generated from a cavity-dumped optical parametric oscillator, synchronously-pumped at 15.3 MHz with sub-400-fs pulses from an Yb:fiber laser. The average beam quality factor of the dumped output was M2 ~1.2 and the total relative-intensity noise was 8 mdBc, making the system a promising candidate for ultrafast laser inscription of infrared materials.

Ultrafast quantum control of ionization dynamics in krypton.

PubMed

Hütten, Konrad; Mittermair, Michael; Stock, Sebastian O; Beerwerth, Randolf; Shirvanyan, Vahe; Riemensberger, Johann; Duensing, Andreas; Heider, Rupert; Wagner, Martin S; Guggenmos, Alexander; Fritzsche, Stephan; Kabachnik, Nikolay M; Kienberger, Reinhard; Bernhardt, Birgitta

2018-02-19

Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump-probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.

A Solution-Processed Ultrafast Optical Switch Based on a Nanostructured Epsilon-Near-Zero Medium.

PubMed

Guo, Qiangbing; Cui, Yudong; Yao, Yunhua; Ye, Yuting; Yang, Yue; Liu, Xueming; Zhang, Shian; Liu, Xiaofeng; Qiu, Jianrong; Hosono, Hideo

2017-07-01

All the optical properties of materials are derived from dielectric function. In spectral region where the dielectric permittivity approaches zero, known as epsilon-near-zero (ENZ) region, the propagating light within the material attains a very high phase velocity, and meanwhile the material exhibits strong optical nonlinearity. The interplay between the linear and nonlinear optical response in these materials thus offers unprecedented pathways for all-optical control and device design. Here the authors demonstrate ultrafast all-optical modulation based on a typical ENZ material of indium tin oxide (ITO) nanocrystals (NCs), accessed by a wet-chemistry route. In the ENZ region, the authors find that the optical response in these ITO NCs is associated with a strong nonlinear character, exhibiting sub-picosecond response time (corresponding to frequencies over 2 THz) and modulation depth up to ≈160%. This large optical nonlinearity benefits from the highly confined geometry in addition to the ENZ enhancement effect of the ITO NCs. Based on these ENZ NCs, the authors successfully demonstrate a fiber optical switch that allows switching of continuous laser wave into femtosecond laser pulses. Combined with facile processibility and tunable optical properties, these solution-processed ENZ NCs may offer a scalable and printable material solution for dynamic photonic and optoelectronic devices. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Direct Absorption Spectroscopy with Electro-Optic Frequency Combs

NASA Astrophysics Data System (ADS)

Fleisher, Adam J.; Long, David A.; Plusquellic, David F.; Hodges, Joseph T.

2017-06-01

The application of electro-optic frequency combs to direct absorption spectroscopy has increased research interest in high-agility, modulator-based comb generation. This talk will review common architectures for electro-optic frequency comb generators as well as describe common self-heterodyne and multi-heterodyne (i.e., dual-comb) detection approaches. In order to achieve a sufficient signal-to-noise ratio on the recorded interferogram while allowing for manageable data volumes, broadband electro-optic frequency combs require deep coherent averaging, preferably in real-time. Applications such as cavity-enhanced spectroscopy, precision atomic and molecular spectroscopy, as well as time-resolved spectroscopy will be introduced. D.A. Long et al., Opt. Lett. 39, 2688 (2014) A.J. Fleisher et al., Opt. Express 24, 10424 (2016)

Ultrafast intersystem-crossing in platinum containing π-conjugated polymers with tunable spin-orbit coupling.

PubMed

Sheng, C-X; Singh, S; Gambetta, A; Drori, T; Tong, M; Tretiak, S; Vardeny, Z V

2013-01-01

The development of efficient organic light-emitting diodes (OLED) and organic photovoltaic cells requires control over the dynamics of spin sensitive excitations. Embedding heavy metal atoms in π-conjugated polymer chains enhances the spin-orbit coupling (SOC), and thus facilitates intersystem crossing (ISC) from the singlet to triplet manifolds. Here we use various nonlinear optical spectroscopies such as two-photon absorption and electroabsorption in conjunction with electronic structure calculations, for studying the energies, emission bands and ultrafast dynamics of spin photoexcitations in two newly synthesized π-conjugated polymers that contain intrachain platinum (Pt) atoms separated by one (Pt-1) or three (Pt-3) organic spacer units. The controllable SOC in these polymers leads to a record ISC time of <~1 ps in Pt-1 and ~6 ps in Pt-3. The tunable ultrafast ISC rate modulates the intensity ratio of the phosphorescence and fluorescence emission bands, with potential applications for white OLEDs.

Extreme nonlinear terahertz electro-optics in diamond for ultrafast pulse switching

NASA Astrophysics Data System (ADS)

Shalaby, Mostafa; Vicario, Carlo; Hauri, Christoph P.

2017-03-01

Polarization switching of picosecond laser pulses is a fundamental concept in signal processing [C. Chen and G. Liu, Annu. Rev. Mater. Sci. 16, 203 (1986); V. R. Almeida et al., Nature 431, 1081 (2004); and A. A. P. Pohl et al., Photonics Sens. 3, 1 (2013)]. Conventional switching devices rely on the electro-optical Pockels effect and work at radio frequencies. The ensuing gating time of several nanoseconds is a bottleneck for faster switches which is set by the performance of state-of-the-art high-voltage electronics. Here we show that by substituting the electric field of several kV/cm provided by modern electronics by the MV/cm field of a single-cycle THz laser pulse, the electro-optical gating process can be driven orders of magnitude faster, at THz frequencies. In this context, we introduce diamond as an exceptional electro-optical material and demonstrate a pulse gating time as fast as 100 fs using sub-cycle THz-induced Kerr nonlinearity. We show that THz-induced switching in the insulator diamond is fully governed by the THz pulse shape. The presented THz-based electro-optical approach overcomes the bandwidth and switching speed limits of conventional MHz/GHz electronics and establishes the ultrafast electro-optical gating technology for the first time in the THz frequency range. We finally show that the presented THz polarization gating technique is applicable for advanced beam diagnostics. As a first example, we demonstrate tomographic reconstruction of a THz pulse in three dimensions.

The perspectives of femtosecond imaging and spectroscopy of complex materials using electrons

NASA Astrophysics Data System (ADS)

Ruan, Chong-Yu; Duxbury, Phiilp M.; Berz, Martin

2014-09-01

The coexistence of various electronic and structural phases that are close in free-energy is a hallmark in strongly correlated electron systems with emergent properties, such as metal-insulator transition, colossal magnetoresistance, and high-temperature superconductivity. The cooperative phase transitions from one functional state to another can involve entanglements between the electronically and structurally ordered states, hence deciphering the fundamental mechanisms is generally difficult and remains very active in condensed matter physics and functional materials research. We outline the recent ultrafast characterizations of 2D charge-density wave materials, including the nonequilibrium electron dynamics unveiled by ultrafast optical spectroscopy-based techniques sensitive to the electronic order parameter. We also describe the most recent findings from ultrafast electron crystallography, which provide structural aspects to correlate lattice dynamics with electronic evolutions to address the two sides of a coin in the ultrafast switching of a cooperative state. Combining these results brings forth new perspectives and a fuller picture in understanding lightmatter interactions and various switching mechanisms in cooperative systems with many potential applications. We also discuss the prospects of implementing new ultrafast electron imaging as a local probe incorporated with femtosecond select-area diffraction, imaging and spectroscopy to provide a full scope of resolution to tackle the more challenging complex phase transitions on the femtosecond-nanometer scale all at once based on a recent understanding of the spacespace- charge-driven emittance limitation on the ultimate performance of these devices. The projection shows promising parameter space for conducting ultrafast electron micordiffraction at close to single-shot level, which is supported by the latest experimental characterization of such a system.

Hyper-Ramsey spectroscopy of optical clock transitions

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

Yudin, V. I.; Taichenachev, A. V.; Oates, C. W.

2010-07-15

We present nonstandard optical Ramsey schemes that use pulses individually tailored in duration, phase, and frequency to cancel spurious frequency shifts related to the excitation itself. In particular, the field shifts and their uncertainties can be radically suppressed (by two to four orders of magnitude) in comparison with the usual Ramsey method (using two equal pulses) as well as with single-pulse Rabi spectroscopy. Atom interferometers and optical clocks based on two-photon transitions, heavily forbidden transitions, or magnetically induced spectroscopy could significantly benefit from this method. In the latter case, these frequency shifts can be suppressed considerably below a fractional levelmore » of 10{sup -17}. Moreover, our approach opens the door for high-precision optical clocks based on direct frequency comb spectroscopy.« less

Ultrafast Graphene Photonics and Optoelectronics

DTIC Science & Technology

2017-04-14

SUBJECT TERMS Graphene, Ultrafast Optical Processin, Terahertz Electronics ; 16. SECURITY CLASSIFICATION OF: 17. LIMITATION OF ABSTRACT SAR 18...Rep, (2016)) Fig. 4. (a) Images of scanning electron microscope for 1D and 2D gratings. (b) Ratio of the real part of the transmitted field

A robust and tuneable mid-infrared optical switch enabled by bulk Dirac fermions.

PubMed

Zhu, Chunhui; Wang, Fengqiu; Meng, Yafei; Yuan, Xiang; Xiu, Faxian; Luo, Hongyu; Wang, Yazhou; Li, Jianfeng; Lv, Xinjie; He, Liang; Xu, Yongbing; Liu, Junfeng; Zhang, Chao; Shi, Yi; Zhang, Rong; Zhu, Shining

2017-01-20

Pulsed lasers operating in the mid-infrared (3-20 μm) are important for a wide range of applications in sensing, spectroscopy, imaging and communications. Despite recent advances with mid-infrared gain platforms, the lack of a capable pulse generation mechanism remains a significant technological challenge. Here we show that bulk Dirac fermions in molecular beam epitaxy grown crystalline Cd 3 As 2 , a three-dimensional topological Dirac semimetal, constitutes an exceptional ultrafast optical switching mechanism for the mid-infrared. Significantly, we show robust and effective tuning of the scattering channels of Dirac fermions via an element doping approach, where photocarrier relaxation times are found flexibly controlled over an order of magnitude (from 8 ps to 800 fs at 4.5 μm). Our findings reveal the strong impact of Cr doping on ultrafast optical properties in Cd 3 As 2 and open up the long sought parameter space crucial for the development of compact and high-performance mid-infrared ultrafast sources.

A robust and tuneable mid-infrared optical switch enabled by bulk Dirac fermions

NASA Astrophysics Data System (ADS)

Zhu, Chunhui; Wang, Fengqiu; Meng, Yafei; Yuan, Xiang; Xiu, Faxian; Luo, Hongyu; Wang, Yazhou; Li, Jianfeng; Lv, Xinjie; He, Liang; Xu, Yongbing; Liu, Junfeng; Zhang, Chao; Shi, Yi; Zhang, Rong; Zhu, Shining

2017-01-01

Pulsed lasers operating in the mid-infrared (3-20 μm) are important for a wide range of applications in sensing, spectroscopy, imaging and communications. Despite recent advances with mid-infrared gain platforms, the lack of a capable pulse generation mechanism remains a significant technological challenge. Here we show that bulk Dirac fermions in molecular beam epitaxy grown crystalline Cd3As2, a three-dimensional topological Dirac semimetal, constitutes an exceptional ultrafast optical switching mechanism for the mid-infrared. Significantly, we show robust and effective tuning of the scattering channels of Dirac fermions via an element doping approach, where photocarrier relaxation times are found flexibly controlled over an order of magnitude (from 8 ps to 800 fs at 4.5 μm). Our findings reveal the strong impact of Cr doping on ultrafast optical properties in Cd3As2 and open up the long sought parameter space crucial for the development of compact and high-performance mid-infrared ultrafast sources.

Structural relaxation in the hydrogen-bonding liquids N-methylacetamide and water studied by optical Kerr effect spectroscopy.

PubMed

Turton, David A; Wynne, Klaas

2008-04-21

Structural relaxation in the peptide model N-methylacetamide (NMA) is studied experimentally by ultrafast optical Kerr effect spectroscopy over the normal-liquid temperature range and compared to the relaxation measured in water at room temperature. It is seen that in both hydrogen-bonding liquids, beta relaxation is present, and in each case, it is found that this can be described by the Cole-Cole function. For NMA in this temperature range, the alpha and beta relaxations are each found to have an Arrhenius temperature dependence with indistinguishable activation energies. It is known that the variations on the Debye function, including the Cole-Cole function, are unphysical, and we introduce two general modifications: One allows for the initial rise of the function, determined by the librational frequencies, and the second allows the function to be terminated in the alpha relaxation.

The Ultrafast Wolff Rearrangement in the Gas Phase

NASA Astrophysics Data System (ADS)

Steinbacher, Andreas; Roeding, Sebastian; Brixner, Tobias; Nuernberger, Patrick

The Wolff rearrangement of gas-phase 5-diazo Meldrum's acid is disclosed with femtosecond ion spectroscopy. Distinct differences are found for 267 nm and 200 nm excitation, the latter leading to even two ultrafast rearrangement reactions.

Ultrafast Spectroscopy of Mid-Infrared Semiconductors Using the Signal and Idler Beams of a Synchronous Optical Parametric Oscillator

DTIC Science & Technology

2008-03-01

then used to fit theoretical models describing radiative and non-radiative relaxation processes. 3.2 Experimental Setup This thesis uses a mode...Russian Efforts. Master’s thesis, Naval Postgraduate School, 2005. 5. Chirsto, Farid C. “Thermochemistry and Kinetics Models for MagnesiumTe- flon/Viton...Coherent Mira Model 900-F Laser. 7. Cooley, William T. Measurement of Ultrafast Carrier Recombination Dynamics in Mid-Infrared Semiconductor Laser Material

Spin-controlled ultrafast vertical-cavity surface-emitting lasers

NASA Astrophysics Data System (ADS)

Höpfner, Henning; Lindemann, Markus; Gerhardt, Nils C.; Hofmann, Martin R.

2014-05-01

Spin-controlled semiconductor lasers are highly attractive spintronic devices providing characteristics superior to their conventional purely charge-based counterparts. In particular, spin-controlled vertical-cavity surface emitting lasers (spin-VCSELs) promise to offer lower thresholds, enhanced emission intensity, spin amplification, full polarization control, chirp control and ultrafast dynamics. Most important, the ability to control and modulate the polarization state of the laser emission with extraordinarily high frequencies is very attractive for many applications like broadband optical communication and ultrafast optical switches. We present a novel concept for ultrafast spin-VCSELs which has the potential to overcome the conventional speed limitation for directly modulated lasers by the relaxation oscillation frequency and to reach modulation frequencies significantly above 100 GHz. The concept is based on the coupled spin-photon dynamics in birefringent micro-cavity lasers. By injecting spin-polarized carriers in the VCSEL, oscillations of the coupled spin-photon system can by induced which lead to oscillations of the polarization state of the laser emission. These oscillations are decoupled from conventional relaxation oscillations of the carrier-photon system and can be much faster than these. Utilizing these polarization oscillations is thus a very promising approach to develop ultrafast spin-VCSELs for high speed optical data communication in the near future. Different aspects of the spin and polarization dynamics, its connection to birefringence and bistability in the cavity, controlled switching of the oscillations, and the limitations of this novel approach will be analysed theoretically and experimentally for spin-polarized VCSELs at room temperature.

Ultrafast transient absorption revisited: Phase-flips, spectral fingers, and other dynamical features

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

Cina, Jeffrey A., E-mail: cina@uoregon.edu; Kovac, Philip A.; Jumper, Chanelle C.

We rebuild the theory of ultrafast transient-absorption/transmission spectroscopy starting from the optical response of an individual molecule to incident femtosecond pump and probe pulses. The resulting description makes use of pulse propagators and free molecular evolution operators to arrive at compact expressions for the several contributions to a transient-absorption signal. In this alternative description, which is physically equivalent to the conventional response-function formalism, these signal contributions are conveniently expressed as quantum mechanical overlaps between nuclear wave packets that have undergone different sequences of pulse-driven optical transitions and time-evolution on different electronic potential-energy surfaces. Using this setup in application to amore » simple, multimode model of the light-harvesting chromophores of PC577, we develop wave-packet pictures of certain generic features of ultrafast transient-absorption signals related to the probed-frequency dependence of vibrational quantum beats. These include a Stokes-shifting node at the time-evolving peak emission frequency, antiphasing between vibrational oscillations on opposite sides (i.e., to the red or blue) of this node, and spectral fingering due to vibrational overtones and combinations. Our calculations make a vibrationally abrupt approximation for the incident pump and probe pulses, but properly account for temporal pulse overlap and signal turn-on, rather than neglecting pulse overlap or assuming delta-function excitations, as are sometimes done.« less

EDITORIAL: Ultrafast magnetization processes

NASA Astrophysics Data System (ADS)

Hillebrands, Burkard

2008-09-01

fields can be used to induce a local demagnetization of the sample following femtosecond laser excitation. A B Schmidt et al [164003] report a new access to the surface electronic structure of fcc Co films combining spin-resolved one- and two-photon photoemission. The knowledge of surface states is important for interpreting time-resolved measurements of ultrafast magnetization dynamics in this material. An extension of ultrafast dynamics has been made by several groups. A Melnikov et al [164004] report on the ultrafast dynamics at lanthanide surfaces such as Gd(0001) and Tb(0001) using time-resolved second-harmonic generation and photoelectron spectroscopy. These surfaces exhibit a rich dynamics including a collective response of the crystal lattice and the magnetization. Effects of phonon-magnon scattering are discussed. M Fiebig et al [164005] report on experiments of ultrafast magnetization dynamics in antiferromagnetic compounds, and show that the magnetization dynamics in these systems differs noticeably from that of ferromagnetic compounds. They use optical second-harmonic generation and linear reflection to monitor the evolution of the antiferromagnetic order parameter subsequent to an intense optical excitation. In a theory paper, the local light-induced spin manipulation in two-magnetic-centre metallic chains is studied by T Hardenstein et al [164006] using highly correlational ab initio calculations. They show that, as an example of local spin manipulation, the spin on the iron side of a Co-Na-Fe cluster can be switched. S Halm et al [164007] present evidence to manipulate spin states in a diluted magnetic semiconductor on a submicrometer length scale via the magnetic fringe fields of micro-structured magnets. By optically switching the magnetization of the ferromagnet, the magnetization in the semiconductor is manipulated and the limits of a dynamical interaction between the spin states in the ferromagnet and the magnetic semiconductor are discussed. A second

Ultrafast FADC multiplexer

NASA Astrophysics Data System (ADS)

Mirzoyan, R.; Cortina, J.; Lorenz, E.; Martinez, M.; Ostankov, A.; Paneque, D.

2002-10-01

Ultrafast Flash amplitude-to-digital converters (FADCs) are still very expensive. Here we propose a multiplexing scheme allowing one in common trigger mode to read out multiple signal sources by using a single FADC channel. Usual coaxial cables can be used in the multiplexer as analog signal delay elements. The limited bandwidth of the coaxial cable, depending on its type and length will set an upper limit to the number of multiplexed channels. Better bandwidth and the correspondingly higher number of multiplexed channels one can obtain when using the technique of transmission of analog signals via optical fibers. Low-cost vertical cavity surface emitting laser (VCSEL) diodes can be used as converters of fast electrical signals into near infrared light. Multiplexing can be an economically priced solution when one needs ultrafast digitization of hundreds of fast signal channels.

Role of surface states and defects in the ultrafast nonlinear optical properties of CuS quantum dots

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

Mary, K. A. Ann; Unnikrishnan, N. V., E-mail: nvu100@yahoo.com; Philip, Reji

2014-07-01

We report facile preparation of water dispersible CuS quantum dots (2–4 nm) and nanoparticles (5–11 nm) through a nontoxic, green, one-pot synthesis method. Optical and microstructural studies indicate the presence of surface states and defects (dislocations, stacking faults, and twins) in the quantum dots. The smaller crystallite size and quantum dot formation have significant effects on the high energy excitonic and low energy plasmonic absorption bands. Effective two-photon absorption coefficients measured using 100 fs laser pulses employing open-aperture Z-scan in the plasmonic region of 800 nm reveal that CuS quantum dots are better ultrafast optical limiters compared to CuS nanoparticles.

Demonstration of Two-Atom Entanglement with Ultrafast Optical Pulses

NASA Astrophysics Data System (ADS)

Wong-Campos, J. D.; Moses, S. A.; Johnson, K. G.; Monroe, C.

2017-12-01

We demonstrate quantum entanglement of two trapped atomic ion qubits using a sequence of ultrafast laser pulses. Unlike previous demonstrations of entanglement mediated by the Coulomb interaction, this scheme does not require confinement to the Lamb-Dicke regime and can be less sensitive to ambient noise due to its speed. To elucidate the physics of an ultrafast phase gate, we generate a high entanglement rate using just ten pulses, each of ˜20 ps duration, and demonstrate an entangled Bell state with (76 ±1 )% fidelity. These results pave the way for entanglement operations within a large collection of qubits by exciting only local modes of motion.

Demonstration of Two-Atom Entanglement with Ultrafast Optical Pulses.

PubMed

Wong-Campos, J D; Moses, S A; Johnson, K G; Monroe, C

2017-12-08

We demonstrate quantum entanglement of two trapped atomic ion qubits using a sequence of ultrafast laser pulses. Unlike previous demonstrations of entanglement mediated by the Coulomb interaction, this scheme does not require confinement to the Lamb-Dicke regime and can be less sensitive to ambient noise due to its speed. To elucidate the physics of an ultrafast phase gate, we generate a high entanglement rate using just ten pulses, each of ∼20  ps duration, and demonstrate an entangled Bell state with (76±1)% fidelity. These results pave the way for entanglement operations within a large collection of qubits by exciting only local modes of motion.

Ultrafast Plasmon-Enhanced Hot Electron Generation at Ag Nanocluster/Graphite Heterojunctions.

PubMed

Tan, Shijing; Liu, Liming; Dai, Yanan; Ren, Jindong; Zhao, Jin; Petek, Hrvoje

2017-05-03

Hot electron processes at metallic heterojunctions are central to optical-to-chemical or electrical energy transduction. Ultrafast nonlinear photoexcitation of graphite (Gr) has been shown to create hot thermalized electrons at temperatures corresponding to the solar photosphere in less than 25 fs. Plasmonic resonances in metallic nanoparticles are also known to efficiently generate hot electrons. Here we deposit Ag nanoclusters (NC) on Gr to study the ultrafast hot electron generation and dynamics in their plasmonic heterojunctions by means of time-resolved two-photon photoemission (2PP) spectroscopy. By tuning the wavelength of p-polarized femtosecond excitation pulses, we find an enhancement of 2PP yields by 2 orders of magnitude, which we attribute to excitation of a surface-normal Mie plasmon mode of Ag/Gr heterojunctions at 3.6 eV. The 2PP spectra include contributions from (i) coherent two-photon absorption of an occupied interface state (IFS) 0.2 eV below the Fermi level, which electronic structure calculations assign to chemisorption-induced charge transfer, and (ii) hot electrons in the π*-band of Gr, which are excited through the coherent screening response of the substrate. Ultrafast pump-probe measurements show that the IFS photoemission occurs via virtual intermediate states, whereas the characteristic lifetimes attribute the hot electrons to population of the π*-band of Gr via the plasmon dephasing. Our study directly probes the mechanisms for enhanced hot electron generation and decay in a model plasmonic heterojunction.

Asymmetric-detection time-stretch optical microscopy (ATOM) for ultrafast high-contrast cellular imaging in flow

PubMed Central

Wong, Terence T. W.; Lau, Andy K. S.; Ho, Kenneth K. Y.; Tang, Matthew Y. H.; Robles, Joseph D. F.; Wei, Xiaoming; Chan, Antony C. S.; Tang, Anson H. L.; Lam, Edmund Y.; Wong, Kenneth K. Y.; Chan, Godfrey C. F.; Shum, Ho Cheung; Tsia, Kevin K.

2014-01-01

Accelerating imaging speed in optical microscopy is often realized at the expense of image contrast, image resolution, and detection sensitivity – a common predicament for advancing high-speed and high-throughput cellular imaging. We here demonstrate a new imaging approach, called asymmetric-detection time-stretch optical microscopy (ATOM), which can deliver ultrafast label-free high-contrast flow imaging with well delineated cellular morphological resolution and in-line optical image amplification to overcome the compromised imaging sensitivity at high speed. We show that ATOM can separately reveal the enhanced phase-gradient and absorption contrast in microfluidic live-cell imaging at a flow speed as high as ~10 m/s, corresponding to an imaging throughput of ~100,000 cells/sec. ATOM could thus be the enabling platform to meet the pressing need for intercalating optical microscopy in cellular assay, e.g. imaging flow cytometry – permitting high-throughput access to the morphological information of the individual cells simultaneously with a multitude of parameters obtained in the standard assay. PMID:24413677

Optical spectroscopy and tooth decay

NASA Astrophysics Data System (ADS)

Misra, P.; De, T.; Singh, R.

2005-11-01

Optical spectroscopy in the ultraviolet, visible and mid-infrared spectral regions has been used to discriminate between healthy and diseased teeth of patients in the age range 15-75 years. Spectral scans of absorbance versus wavenumber and fluorescence intensity versus wavelength have been recorded and investigated for caries and periodontal disease. Such optical diagnostics can prove very useful in the early detection and treatment of tooth decay.

Filter-Based Dispersion-Managed Versatile Ultrafast Fibre Laser

PubMed Central

Peng, Junsong; Boscolo, Sonia

2016-01-01

We present the operation of an ultrafast passively mode-locked fibre laser, in which flexible control of the pulse formation mechanism is readily realised by an in-cavity programmable filter the dispersion and bandwidth of which can be software configured. We show that conventional soliton, dispersion-managed (DM) soliton (stretched-pulse) and dissipative soliton mode-locking regimes can be reliably targeted by changing the filter’s dispersion and bandwidth only, while no changes are made to the physical layout of the laser cavity. Numerical simulations are presented which confirm the different nonlinear pulse evolutions inside the laser cavity. The proposed technique holds great potential for achieving a high degree of control over the dynamics and output of ultrafast fibre lasers, in contrast to the traditional method to control the pulse formation mechanism in a DM fibre laser, which involves manual optimisation of the relative length of fibres with opposite-sign dispersion in the cavity. Our versatile ultrafast fibre laser will be attractive for applications requiring different pulse profiles such as in optical signal processing and optical communications. PMID:27183882

Ultrafast Two-Dimensional Infrared Spectroscopy of a Quasifree Rotor: J Scrambling and Perfectly Anticorrelated Cross Peaks

NASA Astrophysics Data System (ADS)

Mandal, Aritra; Ng Pack, Greg; Shah, Parth P.; Erramilli, Shyamsunder; Ziegler, L. D.

2018-03-01

Ultrafast two-dimensional infrared (2DIR) spectra of the N2O ν3 mode in moderately dense SF6 gas exhibit complex line shapes with diagonal and antidiagonal features in contrast to condensed phase vibrational 2DIR spectroscopy. Observed spectra for this quasifree rotor system are well captured by a model that includes all 36 possible rovibrational pathways and treats P (Δ J =-1 ) and R (Δ J =+1 ) branch resonances as distinct Kubo line shape features. Transition frequency correlation decay is due to J scrambling within one to two gas collisions at each density. Studies of supercritical solvation and relaxation at high pressure and temperature are enabled by this methodology.

Impact of metal ions in porphyrin-based applied materials for visible-light photocatalysis: key information from ultrafast electronic spectroscopy.

PubMed

Kar, Prasenjit; Sardar, Samim; Alarousu, Erkki; Sun, Jingya; Seddigi, Zaki S; Ahmed, Saleh A; Danish, Ekram Y; Mohammed, Omar F; Pal, Samir Kumar

2014-08-11

Protoporphyrin IX-zinc oxide (PP-ZnO) nanohybrids have been synthesized for applications in photocatalytic devices. High-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), and steady-state infrared, absorption, and emission spectroscopies have been used to analyze the structural details and optical properties of these nanohybrids. Time-resolved fluorescence and transient absorption techniques have been applied to study the ultrafast dynamic events that are key to photocatalytic activities. The photocatalytic efficiency under visible-light irradiation in the presence of naturally abundant iron(III) and copper(II) ions has been found to be significantly retarded in the former case, but enhanced in the latter case. More importantly, femtosecond (fs) transient absorption data have clearly demonstrated that the residence of photoexcited electrons from the sensitizer PP in the centrally located iron moiety hinders ground-state bleach recovery of the sensitizer, affecting the overall photocatalytic rate of the nanohybrid. The presence of copper(II) ions, on the other hand, offers additional stability against photobleaching and eventually enhances the efficiency of photocatalysis. In addition, we have also explored the role of UV light in the efficiency of photocatalysis and have rationalized our observations from femtosecond- to picosecond-resolved studies. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Properties of the anion-binding site of pharaonis Halorhodopsin studied by ultrafast pump-probe spectroscopy and low-temperature FTIR spectroscopy.

PubMed

Nakashima, Keisuke; Nakamura, Takumi; Takeuchi, Satoshi; Shibata, Mikihiro; Demura, Makoto; Tahara, Tahei; Kandori, Hideki

2009-06-18

Halorhodopsin (HR) is a light-driven chloride pump. Cl(-) is bound in the Schiff base region of the retinal chromophore, and unidirectional Cl(-) transport is probably enforced by the specific hydrogen-bonding interaction with the protonated Schiff base and internal water molecules. It is known that HR from Natronobacterium pharaonis (pHR) also pumps NO(3)(-) with similar efficiency, suggesting that NO(3)(-) binds to the Cl(-)-binding site. In the present study, we investigated the properties of the anion-binding site by means of ultrafast pump-probe spectroscopy and low-temperature FTIR spectroscopy. The obtained data were surprisingly similar between pHR-NO(3)(-) and pHR-Cl(-), even though the shapes and sizes of the two anions are quite different. Femtosecond pump-probe spectroscopy showed very similar excited-state dynamics between pHR-NO(3)(-) and pHR-Cl(-). Low-temperature FTIR spectroscopy of unlabeled and [zeta-(15)N]Lys-labeled pHR revealed almost identical hydrogen-bonding strengths of the protonated retinal Schiff base between pHR-NO(3)(-) and pHR-Cl(-), which is similarly strengthened after retinal isomerization. There were spectral variations for water stretching vibrations between pHR-NO(3)(-) and pHR-Cl(-), suggesting that the water molecules hydrate each anion. Nevertheless, the overall spectral features were similar for the two species. These observations strongly suggest that the anion-binding site has a flexible structure and that the interaction between retinal and the anions is weak, despite the presence of an electrostatic interaction. Such a flexible hydrogen-bonding network in the Schiff base region in HR appears to be in remarkable contrast to that in light-driven proton-pumping proteins.

Activation of coherent lattice phonon following ultrafast molecular spin-state photo-switching: A molecule-to-lattice energy transfer

PubMed Central

Marino, A.; Cammarata, M.; Matar, S. F.; Létard, J.-F.; Chastanet, G.; Chollet, M.; Glownia, J. M.; Lemke, H. T.; Collet, E.

2015-01-01

We combine ultrafast optical spectroscopy with femtosecond X-ray absorption to study the photo-switching dynamics of the [Fe(PM-AzA)2(NCS)2] spin-crossover molecular solid. The light-induced excited spin-state trapping process switches the molecules from low spin to high spin (HS) states on the sub-picosecond timescale. The change of the electronic state (<50 fs) induces a structural reorganization of the molecule within 160 fs. This transformation is accompanied by coherent molecular vibrations in the HS potential and especially a rapidly damped Fe-ligand breathing mode. The time-resolved studies evidence a delayed activation of coherent optical phonons of the lattice surrounding the photoexcited molecules. PMID:26798836

Ultrafast Spectroscopic Studies of Two-Photon States in Third Order Optical Processes of Dye Chromophores.

NASA Astrophysics Data System (ADS)

Yu, Yi-Zhong

1995-01-01

Conjugated organic and polymeric materials usually have large, nonresonant third order optical nonlinearity due to correlations of their delocalized pi -electrons. Most materials studied so far show positive values of third order nonlinear susceptibility when all frequencies that generate the third order effect are below any optical transition. A new class of organic molecules, namely indole squarylium (ISQ) and anilinium squarylium (BSQ), exhibit negative < gamma(-omega_4;omega_1, omega_2,omega_3)> when all three frequencies, omega_1, omega_2 and omega_3, lie below the first electronic transition. Although quantum many-electron calculations based on multiple-excitation configuration interaction have shown that the negative third order coefficient is essentially due to the contribution from high-lying two-photon states, the field of experimental studies exploring the microscopic origins of the negative squaraines remains uncultivated. The work presented in this thesis involves extensive experimental investigation of squaraines using techniques such as time-resolved transit absorption spectroscopy and saturable absorption. Theoretical simulations studying nonlinear absorption behavior of a simplified two-level system with ultrashort pulses are also presented. Part of the thesis is dedicated to the development, fabrication and characterization of our ultrafast laser system which offers tunable femtosecond pulses at wavelengths from UV to IR and served as a major tool in the experimental measurements. The dynamics of the population inversion between the ground state and the first excited state was also investigated through time-resolved experiments. The experiment results agree well with the theoretical predictions. Strong couplings between the gateway state and high-lying two-photon states were observed in BSQ squarylium molecules, which suggested a complete quantum calculation with multiple energy levels is required to

Ultrafast laser ablation for targeted atherosclerotic plaque removal

NASA Astrophysics Data System (ADS)

Lanvin, Thomas; Conkey, Donald B.; Descloux, Laurent; Frobert, Aurelien; Valentin, Jeremy; Goy, Jean-Jacques; Cook, Stéphane; Giraud, Marie-Noelle; Psaltis, Demetri

2015-07-01

Coronary artery disease, the main cause of heart disease, develops as immune cells and lipids accumulate into plaques within the coronary arterial wall. As a plaque grows, the tissue layer (fibrous cap) separating it from the blood flow becomes thinner and increasingly susceptible to rupturing and causing a potentially lethal thrombosis. The stabilization and/or treatment of atherosclerotic plaque is required to prevent rupturing and remains an unsolved medical problem. Here we show for the first time targeted, subsurface ablation of atherosclerotic plaque using ultrafast laser pulses. Excised atherosclerotic mouse aortas were ablated with ultrafast near-infrared (NIR) laser pulses. The physical damage was characterized with histological sections of the ablated atherosclerotic arteries from six different mice. The ultrafast ablation system was integrated with optical coherence tomography (OCT) imaging for plaque-specific targeting and monitoring of the resulting ablation volume. We find that ultrafast ablation of plaque just below the surface is possible without causing damage to the fibrous cap, which indicates the potential use of ultrafast ablation for subsurface atherosclerotic plaque removal. We further demonstrate ex vivo subsurface ablation of a plaque volume through a catheter device with the high-energy ultrafast pulse delivered via hollow-core photonic crystal fiber.

Raman Spectroscopy of Optically Trapped Single Biological Micro-Particles

PubMed Central

Redding, Brandon; Schwab, Mark J.; Pan, Yong-le

2015-01-01

The combination of optical trapping with Raman spectroscopy provides a powerful method for the study, characterization, and identification of biological micro-particles. In essence, optical trapping helps to overcome the limitation imposed by the relative inefficiency of the Raman scattering process. This allows Raman spectroscopy to be applied to individual biological particles in air and in liquid, providing the potential for particle identification with high specificity, longitudinal studies of changes in particle composition, and characterization of the heterogeneity of individual particles in a population. In this review, we introduce the techniques used to integrate Raman spectroscopy with optical trapping in order to study individual biological particles in liquid and air. We then provide an overview of some of the most promising applications of this technique, highlighting the unique types of measurements enabled by the combination of Raman spectroscopy with optical trapping. Finally, we present a brief discussion of future research directions in the field. PMID:26247952

Low-power, ultrafast, and dynamic all-optical tunable plasmon induced transparency in two stub resonators side-coupled with a plasmonic waveguide system

NASA Astrophysics Data System (ADS)

Wang, Boyun; Zeng, Qingdong; Xiao, Shuyuan; Xu, Chen; Xiong, Liangbin; Lv, Hao; Du, Jun; Yu, Huaqing

2017-11-01

We theoretically and numerically investigate a low-power, ultrafast, and dynamic all-optical tunable plasmon induced transparency (PIT) in two stub resonators side-coupled with a metal-dielectric-metal (MDM) plasmonic waveguide system. The optical Kerr effect is enhanced by the local electromagnetic field of surface plasmon polaritons (SPPs) and the plasmonic waveguide based on graphene-Ag composite material structures with large effective Kerr nonlinear coefficient. An ultrafast response time of the order of 1 ps is reached because of ultrafast carrier relaxation dynamics of graphene. With dynamically tuning the propagation phase of the plasmonic waveguide, π-phase shift of the transmission spectrum in the PIT system is achieved under excitation of a pump light with an intensity as low as 5.8 MW cm-2. The group delay is controlled between 0.14 and 0.67 ps. Moreover, the tunable bandwidth of about 42 nm is obtained. For the indirect coupling between two stub cavities or the phase coupling scheme, the phase shift multiplication effect of the PIT effect is found. All observed schemes are analyzed rigorously through finite-difference time-domain simulations and coupled-mode formalism. This work not only paves the way towards the realization of on-chip integrated nanophotonic devices but also opens the possibility of the construction of ultrahigh-speed information processing chips based on plasmonic circuits.

Metalloprotein entatic control of ligand-metal bonds quantified by ultrafast x-ray spectroscopy

DOE PAGES

Mara, Michael W.; Hadt, Ryan G.; Reinhard, Marco Eli; ...

2017-06-23

The multifunctional protein cytochrome c (cyt c) plays key roles in electron transport and apoptosis, switching function by modulating bonding between a heme iron and the sulfur in a methionine residue. This Fe–S(Met) bond is too weak to persist in the absence of protein constraints. We ruptured the bond in ferrous cyt c using an optical laser pulse and monitored the bond reformation within the protein active site using ultrafast x-ray pulses from an x-ray free-electron laser, determining that the Fe–S(Met) bond enthalpy is ~4 kcal/mol stronger than in the absence of protein constraints. As a result, the 4 kcal/molmore » is comparable with calculations of stabilization effects in other systems, demonstrating how biological systems use an entatic state for modest yet accessible energetics to modulate chemical function.« less

Metalloprotein entatic control of ligand-metal bonds quantified by ultrafast x-ray spectroscopy

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

Mara, Michael W.; Hadt, Ryan G.; Reinhard, Marco Eli

The multifunctional protein cytochrome c (cyt c) plays key roles in electron transport and apoptosis, switching function by modulating bonding between a heme iron and the sulfur in a methionine residue. This Fe–S(Met) bond is too weak to persist in the absence of protein constraints. We ruptured the bond in ferrous cyt c using an optical laser pulse and monitored the bond reformation within the protein active site using ultrafast x-ray pulses from an x-ray free-electron laser, determining that the Fe–S(Met) bond enthalpy is ~4 kcal/mol stronger than in the absence of protein constraints. As a result, the 4 kcal/molmore » is comparable with calculations of stabilization effects in other systems, demonstrating how biological systems use an entatic state for modest yet accessible energetics to modulate chemical function.« less

Ultrafast Dynamics of Energetic Materials

DTIC Science & Technology

2014-01-23

redistributed in condensed-phase materials. In this subproject we developed a technique termed three-dimensional IR- Raman spectroscopy that allowed us to...Fang, 2011, “The distribution of local enhancement factors in surface enhanced Raman -active substrates and the vibrational dynamics in the liquid phase...3. (invited) “Vibrational energy and molecular thermometers in liquids: Ultrafast IR- Raman spectroscopy”, Brandt C. Pein and Dana D. Dlott, To

Shift in Chemical Potential of Superconducting Bi2212 Measured by Ultrafast Photoemission Spectroscopy

NASA Astrophysics Data System (ADS)

Miller, Tristan; Smallwood, Chris; Zhang, Wentao; Eisaki, Hiroshi; Lee, Dung-Hai; Lanzara, Alessandra

2015-03-01

Time- and Angle-resolved photoemission spectroscopy (tr-ARPES) has been used to directly measure the dynamics of many different properties of high-temperature superconductors, including the quasiparticle relaxation, cooper pair recombination, and many-body interactions. There have also been several intriguing results on several materials showing how laser pulses can manipulate their chemical potential on ultrafast timescales, and it's been suggested that these effects could find applications in optoelectronic devices. Studies on GaAs have also found that laser pulses may induce a surface voltage effect. Here, we extend these studies for the first time to a Bi2212 sample in the superconducting state, and disentangle the shift in chemical potential from surface voltage effects. This work was supported by Berkeley Lab's program on Quantum Materials, funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-05CH11231.

Cone penetrometer fiber optic raman spectroscopy probe assembly

DOEpatents

Kyle, Kevin R.; Brown, Steven B.

2000-01-01

A chemically and mechanically robust optical Raman spectroscopy probe assembly that can be incorporated in a cone penetrometer (CPT) for subsurface deployment. This assembly consists of an optical Raman probe and a penetrometer compatible optical probe housing. The probe is intended for in-situ chemical analysis of chemical constituents in the surrounding environment. The probe is optically linked via fiber optics to the light source and the detection system at the surface. A built-in broadband light source provides a strobe method for direct measurement of sample optical density. A mechanically stable sapphire window is sealed directly into the side-wall of the housing using a metallic, chemically resistant, hermetic seal design. This window permits transmission of the interrogation light beam and the resultant signal. The spectroscopy probe assembly is capable of accepting Raman, Laser induced Fluorescence, reflectance, and other optical probes with collimated output for CPT deployment.

innoFSPEC: fiber optical spectroscopy and sensing

NASA Astrophysics Data System (ADS)

Roth, Martin M.; Löhmannsröben, Hans-Gerd; Kelz, Andreas; Kumke, Michael

2008-07-01

innoFSPEC Potsdam is presently being established as in interdisciplinary innovation center for fiber-optical spectroscopy and sensing, hosted by Astrophysikalisches Institut Potsdam and the Physical Chemistry group of Potsdam University, Germany. The center focuses on fundamental research in the two fields of fiber-coupled multi-channel spectroscopy and optical fiber-based sensing. Thanks to its interdisciplinary approach, the complementary methodologies of astrophysics on the one hand, and physical chemistry on the other hand, are expected to spawn synergies that otherwise would not normally become available in more standard research programmes. innoFSPEC targets future innovations for next generation astrophysical instrumentation, environmental analysis, manufacturing control and process monitoring, medical diagnostics, non-invasive imaging spectroscopy, biopsy, genomics/proteomics, high-throughput screening, and related applications.

A robust and tuneable mid-infrared optical switch enabled by bulk Dirac fermions

PubMed Central

Zhu, Chunhui; Wang, Fengqiu; Meng, Yafei; Yuan, Xiang; Xiu, Faxian; Luo, Hongyu; Wang, Yazhou; Li, Jianfeng; Lv, Xinjie; He, Liang; Xu, Yongbing; Liu, Junfeng; Zhang, Chao; Shi, Yi; Zhang, Rong; Zhu, Shining

2017-01-01

Pulsed lasers operating in the mid-infrared (3–20 μm) are important for a wide range of applications in sensing, spectroscopy, imaging and communications. Despite recent advances with mid-infrared gain platforms, the lack of a capable pulse generation mechanism remains a significant technological challenge. Here we show that bulk Dirac fermions in molecular beam epitaxy grown crystalline Cd3As2, a three-dimensional topological Dirac semimetal, constitutes an exceptional ultrafast optical switching mechanism for the mid-infrared. Significantly, we show robust and effective tuning of the scattering channels of Dirac fermions via an element doping approach, where photocarrier relaxation times are found flexibly controlled over an order of magnitude (from 8 ps to 800 fs at 4.5 μm). Our findings reveal the strong impact of Cr doping on ultrafast optical properties in Cd3As2 and open up the long sought parameter space crucial for the development of compact and high-performance mid-infrared ultrafast sources. PMID:28106037

Double-Wall Carbon Nanotubes for Wide-Band, Ultrafast Pulse Generation

PubMed Central

2014-01-01

We demonstrate wide-band ultrafast optical pulse generation at 1, 1.5, and 2 μm using a single-polymer composite saturable absorber based on double-wall carbon nanotubes (DWNTs). The freestanding optical quality polymer composite is prepared from nanotubes dispersed in water with poly(vinyl alcohol) as the host matrix. The composite is then integrated into ytterbium-, erbium-, and thulium-doped fiber laser cavities. Using this single DWNT–polymer composite, we achieve 4.85 ps, 532 fs, and 1.6 ps mode-locked pulses at 1066, 1559, and 1883 nm, respectively, highlighting the potential of DWNTs for wide-band ultrafast photonics. PMID:24735347

Quantum and semiclassical physics behind ultrafast optical nonlinearity in the midinfrared: the role of ionization dynamics within the field half cycle.

PubMed

Serebryannikov, E E; Zheltikov, A M

2014-07-25

Ultrafast ionization dynamics within the field half cycle is shown to be the key physical factor that controls the properties of optical nonlinearity as a function of the carrier wavelength and intensity of a driving laser field. The Schrödinger-equation analysis of a generic hydrogen quantum system reveals universal tendencies in the wavelength dependence of optical nonlinearity, shedding light on unusual properties of optical nonlinearities in the midinfrared. For high-intensity low-frequency fields, free-state electrons are shown to dominate over bound electrons in the overall nonlinear response of a quantum system. In this regime, semiclassical models are shown to offer useful insights into the physics behind optical nonlinearity.

Ultrafast Plasmonic Control of Second Harmonic Generation

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

Davidson, Roderick B.; Yanchenko, Anna; Ziegler, Jed I.

Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast control pulse is used to control plasmon-induced electric fields in a thin-film material with inversion symmetry that, without plasmonic enhancement, does not exhibit an even-order nonlinear optical response. The temporal evolution of the plasmonic near-fieldmore » is characterized with ~100 as resolution using a novel nonlinear interferometric technique. The serrated nanogap is a unique platform in which to investigate optically controlled, plasmonically enhanced harmonic generation in dielectric materials on an ultrafast time scale. Lastly, this metamaterial geometry can also be readily extended to all-optical control of other nonlinear phenomena, such as four-wave mixing and sum- and difference-frequency generation, in a wide variety of dielectric materials.« less

Ultrafast Plasmonic Control of Second Harmonic Generation

DOE PAGES

Davidson, Roderick B.; Yanchenko, Anna; Ziegler, Jed I.; ...

2016-06-01

Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast control pulse is used to control plasmon-induced electric fields in a thin-film material with inversion symmetry that, without plasmonic enhancement, does not exhibit an even-order nonlinear optical response. The temporal evolution of the plasmonic near-fieldmore » is characterized with ~100 as resolution using a novel nonlinear interferometric technique. The serrated nanogap is a unique platform in which to investigate optically controlled, plasmonically enhanced harmonic generation in dielectric materials on an ultrafast time scale. Lastly, this metamaterial geometry can also be readily extended to all-optical control of other nonlinear phenomena, such as four-wave mixing and sum- and difference-frequency generation, in a wide variety of dielectric materials.« less

Applications of terahertz spectroscopy and imaging

NASA Astrophysics Data System (ADS)

Zhang, Cunlin; Mu, Kaijun

2009-07-01

We have examined application feasibility of THz time-domain spectroscopy (THz-TDS) to inspect 30 kinds of illicit drugs, 20 kinds of amino acid and 10 kinds of explosives and related compounds (ERCs). We also have got their fingerprints, established the corresponding database, and propose the reference-free methods to extract the absorption or reflection spectra, respectively. We also use optical pump THz probe to research the ultrafast dynamics of semiconductor. While, we also present some new THz imaging techniques, such as, focal-plane multiwavelength phase imaging, reference-free phase imaging, polarization imaging, and continuous-wave (CW) standoff distance imaging.

Plasmonic antennas as design elements for coherent ultrafast nanophotonics.

PubMed

Brinks, Daan; Castro-Lopez, Marta; Hildner, Richard; van Hulst, Niek F

2013-11-12

Broadband excitation of plasmons allows control of light-matter interaction with nanometric precision at femtosecond timescales. Research in the field has spiked in the past decade in an effort to turn ultrafast plasmonics into a diagnostic, microscopy, computational, and engineering tool for this novel nanometric-femtosecond regime. Despite great developments, this goal has yet to materialize. Previous work failed to provide the ability to engineer and control the ultrafast response of a plasmonic system at will, needed to fully realize the potential of ultrafast nanophotonics in physical, biological, and chemical applications. Here, we perform systematic measurements of the coherent response of plasmonic nanoantennas at femtosecond timescales and use them as building blocks in ultrafast plasmonic structures. We determine the coherent response of individual nanoantennas to femtosecond excitation. By mixing localized resonances of characterized antennas, we design coupled plasmonic structures to achieve well-defined ultrafast and phase-stable field dynamics in a predetermined nanoscale hotspot. We present two examples of the application of such structures: control of the spectral amplitude and phase of a pulse in the near field, and ultrafast switching of mutually coherent hotspots. This simple, reproducible and scalable approach transforms ultrafast plasmonics into a straightforward tool for use in fields as diverse as room temperature quantum optics, nanoscale solid-state physics, and quantum biology.

Brillouin micro-spectroscopy through aberrations via sensorless adaptive optics

NASA Astrophysics Data System (ADS)

Edrei, Eitan; Scarcelli, Giuliano

2018-04-01

Brillouin spectroscopy is a powerful optical technique for non-contact viscoelastic characterizations which has recently found applications in three-dimensional mapping of biological samples. Brillouin spectroscopy performances are rapidly degraded by optical aberrations and have therefore been limited to homogenous transparent samples. In this work, we developed an adaptive optics (AO) configuration designed for Brillouin scattering spectroscopy to engineer the incident wavefront and correct for aberrations. Our configuration does not require direct wavefront sensing and the injection of a "guide-star"; hence, it can be implemented without the need for sample pre-treatment. We used our AO-Brillouin spectrometer in aberrated phantoms and biological samples and obtained improved precision and resolution of Brillouin spectral analysis; we demonstrated 2.5-fold enhancement in Brillouin signal strength and 1.4-fold improvement in axial resolution because of the correction of optical aberrations.

Spin-vibronic quantum dynamics for ultrafast excited-state processes.

PubMed

Eng, Julien; Gourlaouen, Christophe; Gindensperger, Etienne; Daniel, Chantal

2015-03-17

Ultrafast intersystem crossing (ISC) processes coupled to nuclear relaxation and solvation dynamics play a central role in the photophysics and photochemistry of a wide range of transition metal complexes. These phenomena occurring within a few hundred femtoseconds are investigated experimentally by ultrafast picosecond and femtosecond transient absorption or luminescence spectroscopies, and optical laser pump-X-ray probe techniques using picosecond and femtosecond X-ray pulses. The interpretation of ultrafast structural changes, time-resolved spectra, quantum yields, and time scales of elementary processes or transient lifetimes needs robust theoretical tools combining state-of-the-art quantum chemistry and developments in quantum dynamics for solving the electronic and nuclear problems. Multimode molecular dynamics beyond the Born-Oppenheimer approximation has been successfully applied to many small polyatomic systems. Its application to large molecules containing a transition metal atom is still a challenge because of the nuclear dimensionality of the problem, the high density of electronic excited states, and the spin-orbit coupling effects. Rhenium(I) α-diimine carbonyl complexes, [Re(L)(CO)3(N,N)](n+) are thermally and photochemically robust and highly flexible synthetically. Structural variations of the N,N and L ligands affect the spectroscopy, the photophysics, and the photochemistry of these chromophores easily incorporated into a complex environment. Visible light absorption opens the route to a wide range of applications such as sensors, probes, or emissive labels for imaging biomolecules. Halide complexes [Re(X)(CO)3(bpy)] (X = Cl, Br, or I; bpy = 2,2'-bipyridine) exhibit complex electronic structure and large spin-orbit effects that do not correlate with the heavy atom effects. Indeed, the (1)MLCT → (3)MLCT intersystem crossing (ISC) kinetics is slower than in [Ru(bpy)3](2+) or [Fe(bpy)3](2+) despite the presence of a third-row transition metal

Ultrafast Fabry-Perot fiber-optic pressure sensors for multimedia blast event measurements.

PubMed

Zou, Xiaotian; Wu, Nan; Tian, Ye; Zhang, Yang; Fitek, John; Maffeo, Michael; Niezrecki, Christopher; Chen, Julie; Wang, Xingwei

2013-02-20

A shock wave (SW) is characterized as a large pressure fluctuation that typically lasts only a few milliseconds. On the battlefield, SWs pose a serious threat to soldiers who are exposed to explosions, which may lead to blast-induced traumatic brain injuries. SWs can also be used beneficially and have been applied to a variety of medical treatments due to their unique interaction with tissues and cells. Consequently, it is important to have sensors that can quantify SW dynamics in order to better understand the physical interaction between body tissue and the incident acoustic wave. In this paper, the ultrafast fiber-optic sensor based on the Fabry-Perot interferometric principle was designed and four such sensors were fabricated to quantify a blast event within different media, simultaneously. The compact design of the fiber-optic sensor allows for a high degree of spatial resolution when capturing the wavefront of the traveling SW. Several blast event experiments were conducted within different media (e.g., air, rubber membrane, and water) to evaluate the sensor's performance. This research revealed valuable knowledge for further study of SW behavior and SW-related applications.

Ultrafast fluorescence spectroscopy via upconversion applications to biophysics.

PubMed

Xu, Jianhua; Knutson, Jay R

2008-01-01

This chapter reviews basic concepts of nonlinear fluorescence upconversion, a technique whose temporal resolution is essentially limited only by the pulse width of the ultrafast laser. Design aspects for upconversion spectrophotofluorometers are discussed, and a recently developed system is described. We discuss applications in biophysics, particularly the measurement of time-resolved fluorescence spectra of proteins (with subpicosecond time resolution). Application of this technique to biophysical problems such as dynamics of tryptophan, peptides, proteins, and nucleic acids is reviewed.

Proceedings of "Optical Probes of Dynamics in Complex Environments"

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

Sension, R; Tokmakoff, A

2008-04-01

This document contains the proceedings from the symposium on Optical Probes of Dynamics in Complex Environments, which organized as part of the 235th National Meeting of the American Chemical Society in New Orleans, LA from April 6 to 10, 2008. The study of molecular dynamics in chemical reaction and biological processes using time ƒresolved spectroscopy plays an important role in our understanding of energy conversion, storage, and utilization problems. Fundamental studies of chemical reactivity, molecular rearrangements, and charge transport are broadly supported by the DOE Office of Science because of their role in the development of alternative energy sources, themore » understanding of biological energy conversion processes, the efficient utilization of existing energy resources, and the mitigation of reactive intermediates in radiation chemistry. In addition, time resolved spectroscopy is central to all of DOEs grand challenges for fundamental energy science. This symposium brought together leaders in the field of ultrafast spectroscopy, including experimentalists, theoretical chemists, and simulators, to discuss the most recent scientific and technological advances. DOE support for this conference was used to help young US and international scientists travel to the meeting. The latest technology in ultrafast infrared, optical, and xray spectroscopy and the scientific advances that these methods enable were covered. Particular emphasis was placed on new experimental methods used to probe molecular dynamics in liquids, solids, interfaces, nanostructured materials, and biomolecules.« less

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.

Ultrafast carrier thermalization and trapping in silicon-germanium alloy probed by extreme ultraviolet transient absorption spectroscopy

PubMed Central

Zürch, Michael; Chang, Hung-Tzu; Kraus, Peter M.; Cushing, Scott K.; Borja, Lauren J.; Gandman, Andrey; Kaplan, Christopher J.; Oh, Myoung Hwan; Prell, James S.; Prendergast, David; Pemmaraju, Chaitanya D.; Neumark, Daniel M.; Leone, Stephen R.

2017-01-01

Semiconductor alloys containing silicon and germanium are of growing importance for compact and highly efficient photonic devices due to their favorable properties for direct integration into silicon platforms and wide tunability of optical parameters. Here, we report the simultaneous direct and energy-resolved probing of ultrafast electron and hole dynamics in a silicon-germanium alloy with the stoichiometry Si0.25Ge0.75 by extreme ultraviolet transient absorption spectroscopy. Probing the photoinduced dynamics of charge carriers at the germanium M4,5-edge (∼30 eV) allows the germanium atoms to be used as reporter atoms for carrier dynamics in the alloy. The photoexcitation of electrons across the direct and indirect band gap into conduction band (CB) valleys and their subsequent hot carrier relaxation are observed and compared to pure germanium, where the Ge direct (ΔEgap,Ge,direct=0.8 eV) and Si0.25Ge0.75 indirect gaps (ΔEgap,Si0.25Ge0.75,indirect=0.95 eV) are comparable in energy. In the alloy, comparable carrier lifetimes are observed for the X, L, and Γ valleys in the conduction band. A midgap feature associated with electrons accumulating in trap states near the CB edge following intraband thermalization is observed in the Si0.25Ge0.75 alloy. The successful implementation of the reporter atom concept for capturing the dynamics of the electronic bands by site-specific probing in solids opens a route to study carrier dynamics in more complex materials with femtosecond and sub-femtosecond temporal resolution. PMID:28653020

Four-Dimensional Ultrafast Electron Microscopy: Insights into an Emerging Technique.

PubMed

Adhikari, Aniruddha; Eliason, Jeffrey K; Sun, Jingya; Bose, Riya; Flannigan, David J; Mohammed, Omar F

2017-01-11

Four-dimensional ultrafast electron microscopy (4D-UEM) is a novel analytical technique that aims to fulfill the long-held dream of researchers to investigate materials at extremely short spatial and temporal resolutions by integrating the excellent spatial resolution of electron microscopes with the temporal resolution of ultrafast femtosecond laser-based spectroscopy. The ingenious use of pulsed photoelectrons to probe surfaces and volumes of materials enables time-resolved snapshots of the dynamics to be captured in a way hitherto impossible by other conventional techniques. The flexibility of 4D-UEM lies in the fact that it can be used in both the scanning (S-UEM) and transmission (UEM) modes depending upon the type of electron microscope involved. While UEM can be employed to monitor elementary structural changes and phase transitions in samples using real-space mapping, diffraction, electron energy-loss spectroscopy, and tomography, S-UEM is well suited to map ultrafast dynamical events on materials surfaces in space and time. This review provides an overview of the unique features that distinguish these techniques and also illustrates the applications of both S-UEM and UEM to a multitude of problems relevant to materials science and chemistry.

Ultrafast structural and electronic dynamics of the metallic phase in a layered manganite

PubMed Central

Piazza, L.; Ma, C.; Yang, H. X.; Mann, A.; Zhu, Y.; Li, J. Q.; Carbone, F.

2013-01-01

The transition between different states in manganites can be driven by various external stimuli. Controlling these transitions with light opens the possibility to investigate the microscopic path through which they evolve. We performed femtosecond (fs) transmission electron microscopy on a bi-layered manganite to study its response to ultrafast photoexcitation. We show that a photoinduced temperature jump launches a pressure wave that provokes coherent oscillations of the lattice parameters, detected via ultrafast electron diffraction. Their impact on the electronic structure are monitored via ultrafast electron energy loss spectroscopy, revealing the dynamics of the different orbitals in response to specific structural distortions. PMID:26913564

Towards Direct Measurement of Ultrafast Vibrational Energy Flow in Proteins

NASA Astrophysics Data System (ADS)

Müller-Werkmeister, Henrike M.; Essig, Martin; Durkin, Patrick; Budisa, Nediljko; Bredenbeck, Jens

Vibrational energy transfer (VET) within a molecule can be investigated in great detail with ultrafast IR spectroscopy. We report on progress towards mapping of VET pathways in proteins using unnatural amino acids as site-specific probes.

Structural dynamics inside a functionalized metal–organic framework probed by ultrafast 2D IR spectroscopy

DOE PAGES

Nishida, Jun; Tamimi, Amr; Fei, Honghan; ...

2014-12-15

One key property of metal-organic frameworks (MOFs) are their structural elasticity. IHere we show that 2D IR spectroscopy with pulse-shaping techniques can probe the ultrafast structural fluctuations of MOFs. 2D IR data, obtained from a vibrational probe attached to the linkers of UiO-66 MOF in low concentration, revealed that the structural fluctuations have time constants of 7 and 670 ps with no solvent. Filling the MOF pores with dimethylformamide (DMF) slows the structural fluctuations by reducing the ability of the MOF to undergo deformations, and the dynamics of the DMF molecules are also greatly restricted. Finally, methodology advances were requiredmore » to remove the severe light scattering caused by the macroscopic-sized MOF particles, eliminate interfering oscillatory components from the 2D IR data, and address Förster vibrational excitation transfer.« less

Ultrafast pre-breakdown dynamics in Al₂O₃SiO₂ reflector by femtosecond UV laser spectroscopy.

PubMed

Du, Juan; Li, Zehan; Xue, Bing; Kobayashi, Takayoshi; Han, Dongjia; Zhao, Yuanan; Leng, Yuxin

2015-06-29

Ultrafast carrier dynamics in Al2O3/SiO2 high reflectors has been investigated by UV femtosecond laser. It is identified by laser spectroscopy that, the carrier dynamics contributed from the front few layers of Al2O3 play a dominating role in the initial laser-induced damage of the UV reflector. Time-resolved reflection decrease after the UV excitation is observed, and conduction electrons is found to relaxed to a mid-gap defect state locating about one photon below the conduction band . To interpret the laser induced carrier dynamics further, a theoretical model including electrons relaxation to a mid-gap state is built, and agrees very well with the experimental results.. To the best of our knowledge, this is the first study on the pre-damage dynamics in UV high reflector induced by femtosecond UV laser.

Plasmonic Antennas for Optical Nanocrystallography and Femtosecond Spatio-Temporal Control

NASA Astrophysics Data System (ADS)

Berweger, Samuel

Controlling optical fields on nanometer length scales has been a long standing problem in optics, driven by the desire to image spatial inhomogeneities of condensed matter on the natural length scales of molecular, electronic, or lattice correlations. The concept of optical antennas based on plasmon resonant nanostructures has emerged as an attractive solution for concentrating and confining light to the nanoscale with a high degree of spatial confinement achieved in the evanescent field. This dissertation focuses on the fundamental characteristics of the antenna properties of plasmonic metal tips and their application for nanometer-resolved optical scanning probe spectroscopy and imaging. First this work demonstrates the extension of tip-enhanced Raman scattering (TERS) to optical nanocrystallography in order to study ferroelectric domain order by using the symmetry selective Raman selection rules for polar phonon modes in combination with the polarization-dependent TERS enhancement. After the derivation of the polar phonon TERS selection rules, ferroelectric domains arising from finite size effects within individual BaTiO3 nanorods are imaged. The second part of this work explores the fundamental characteristics and applications of adiabatic surface plasmon polariton (SPP) nanofocusing as an optical antenna for far- to near-field mode transformation. This process, resulting from the radius-dependent index of refraction experienced by SPP's propagating on tapered waveguides, is shown to result in a nanoconfined optical excitation at the apex of Au tips 10's of nm in size. To demonstrate the general application for background-free spectroscopy, adiabatic nanofocusing TERS is shown to improve contrast and sensitivity, and enables the extension to the near-IR spectral range. Lastly, due to the phase, wavelength, and amplitude independent nanofocusing mechanism, the independent and simultaneous nanometer-femtosecond spatio-temporal control of ultrafast pulses is

Ultrafast Fluorescence Spectroscopy via Upconversion: Applications to Biophysics

PubMed Central

Xu, Jianhua; Knutson, Jay R.

2012-01-01

This chapter reviews basic concepts of nonlinear fluorescence upconversion, a technique whose temporal resolution is essentially limited only by the pulse width of the ultrafast laser. Design aspects for upconversion spectrophotofluorometers are discussed, and a recently developed system is described. We discuss applications in biophysics, particularly the measurement of time-resolved fluorescence spectra of proteins (with subpicosecond time resolution). Application of this technique to biophysical problems such as dynamics of tryptophan, peptides, proteins, and nucleic acids is reviewed. PMID:19152860

Ultrafast time-resolved photoemission of a metallic tip/substrate junction

NASA Astrophysics Data System (ADS)

Meng, Xiang; Jin, Wencan; Yang, Hao; Dadap, Jerry; Osgood, Richard; Camillone, Nicholas, III

The strong near-field enhancement of metallic-tip nanostructures has attracted great interest in scanning microscopy techniques, such as surface-enhanced Raman scattering, near-field scanning optical microscopy and tip-enhanced nonlinear imaging. In this talk, we use a full vectorial 3D-FDTD method to investigate the spatial characteristics of the optical field confinement and localization between a tungsten nanoprobe and an infinite planar silver substrate, with two-color ultrafast laser excitation scheme. The degree of two-color excited field enhancement, geometry dependence, the exact mechanism of optical tip-substrate coupling and tip-substrate plasmon resonances are significant in understanding the electrodynamical responses at tip-substrate junction. The demonstrated measurements with subpicosecond time and subnanometer spatial resolution suggest a new approach to ultrafast time-resolved measurements of surface electron dynamics. DE-FG 02-90-ER-14104; DE-FG 02-04-ER-46157.

Ultrafast Phenomena XIV

NASA Astrophysics Data System (ADS)

Kobayashi, Takayoshi; Okada, Tadashi; Kobayashi, Tetsuro; Nelson, Keith A.; de Silvestri, Sandro

Ultrafast Phenomena XIV presents the latest advances in ultrafast science, including ultrafast laser and measurement technology as well as studies of ultrafast phenomena. Pico-, femto-, and atosecond processes relevant in physics, chemistry, biology, and engineering are presented. Ultrafast technology is now having a profound impact within a wide range of applications, among them imaging, material diagnostics, and transformation and high-speed optoelectronics . This book summarizes results presented at the 14th Ultrafast Phenomena Conference and reviews the state of the art in this important and rapidly advancing field.

The effect of excitation intensity variation and silver nanoparticle codoping on nonlinear optical properties of mixed tellurite and zinc oxide glass doped with Nd2O3 studied through ultrafast z-scan spectroscopy

NASA Astrophysics Data System (ADS)

Moreira, L.; Falci, R. F.; Darabian, H.; Anjos, V.; Bell, M. J. V.; Kassab, L. R. P.; Bordon, C. D. S.; Doualan, J. L.; Camy, P.; Moncorgé, R.

2018-05-01

The research on Nd3+ doped new solid-state laser hosts with specific thermo-mechanical and optical properties is very active. Nd3+ doped tellurite glasses are suitable for these applications. They have high linear and nonlinear refraction index, wide transmittance range. The TeO2-ZnO (TZO) glass considered in the present work combines all those features and the nonlinear optical properties can be used for the development of Kerr-lens mode-locked sub picosecond lasers. Recently the laser performance of Nd3+ doped TZO glass and was reported and laser slope efficiency of 21% was observed. We investigate how the intensity variation and the silver nanoparticles codoping affects the nonlinear optical properties of Nd3+ doped TZO glasses. Intensity dependent nonlinear refraction indices coefficients at 750, 800 and 850 nm were observed. The nonlinear optical features were obtained through ultrafast single beam z-scan technique with excitations at 750, 800 and 850 nm and are up to two orders of magnitude higher than those reported in the literature.

Ultrafast Transient Absorption Spectroscopy of Polymer-Based Organophotoredox Catalysts Mimicking Transition-Metal Complexes

NASA Astrophysics Data System (ADS)

Jamhawi, Abdelqader; Paul, Anam C.; Smith, Justin D.; Handa, Sachin; Liu, Jinjun

2017-06-01

Transition-metal complexes of rare earth metals including ruthenium and iridium are most commonly employed as visible-light photocatalysts. Despite their highly important and broad applications, they have many disadvantages including high cost associated with low abundance in earth crust, potential toxicity, requirement of specialized ligands for desired activity, and difficulty in recycling of metal contents as well as associated ligands. Polymer-based organophotoredox catalysts are promising alternatives and possess unique advantages such as easier synthesis from inexpensive starting material, longer excited state life time, broad range of activity, sustainability, and recyclability. In this research talk, time-resolved photoluminescence and femtosecond transient absorption (TA) spectroscopy measurements of three novel polymer-based organophotoredox catalysts will be presented. By our synthetic team, their catalytic activity has been proven in some highly valuable chemical transformations, that otherwise require transition metal complexes. Time-resolved spectroscopic investigations have demonstrated that photoinduced processes in these catalysts are similar to the transition metal complexes. Especially, intramolecular vibrational relaxation, internal conversion, and intersystem crossing from the S1 state to the T1 state all occur on a sub-picosecond timescale. The long lifetime of the T1 state ( 2-3 microsecond) renders these polymers potent oxidizing and reducing agents. A spectroscopic and kinetic model has been developed for global fitting of TA spectra in both the frequency and time domains. Implication of the current ultrafast spectroscopy studies of these novel molecules to their roles in photocatalysis will be discussed.

Monitoring one-electron photo-oxidation of guanine in DNA crystals using ultrafast infrared spectroscopy

NASA Astrophysics Data System (ADS)

Hall, James P.; Poynton, Fergus E.; Keane, Páraic M.; Gurung, Sarah P.; Brazier, John A.; Cardin, David J.; Winter, Graeme; Gunnlaugsson, Thorfinnur; Sazanovich, Igor V.; Towrie, Michael; Cardin, Christine J.; Kelly, John M.; Quinn, Susan J.

2015-12-01

To understand the molecular origins of diseases caused by ultraviolet and visible light, and also to develop photodynamic therapy, it is important to resolve the mechanism of photoinduced DNA damage. Damage to DNA bound to a photosensitizer molecule frequently proceeds by one-electron photo-oxidation of guanine, but the precise dynamics of this process are sensitive to the location and the orientation of the photosensitizer, which are very difficult to define in solution. To overcome this, ultrafast time-resolved infrared (TRIR) spectroscopy was performed on photoexcited ruthenium polypyridyl-DNA crystals, the atomic structure of which was determined by X-ray crystallography. By combining the X-ray and TRIR data we are able to define both the geometry of the reaction site and the rates of individual steps in a reversible photoinduced electron-transfer process. This allows us to propose an individual guanine as the reaction site and, intriguingly, reveals that the dynamics in the crystal state are quite similar to those observed in the solvent medium.

Ultrafast Absorption Spectroscopy of Aluminum Plasmas Created by LCLS using Betatron X-Ray Radiation

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

Albert, Felicie

2016-10-12

This document summarizes the goals and accomplishments of a six month-long LDRD project, awarded through the LLNL director Early and Mid Career Recognition (EMCR) program. This project allowed us to support beamtime awarded at the Matter under Extreme Conditions (MEC) end station of the Linac Coherent Light Source (LCLS). The goal of the experiment was to heat metallic samples with the bright x-rays from the LCLS free electron laser. Then, we studied how they relaxed back to equilibrium by probing them with ultrafast x-ray absorption spectroscopy using laser-based betatron radiation. Our work enabled large collaborations between LLNL, SLAC, LBNL, andmore » institutions in France and in the UK, while providing training to undergraduate and graduate students during the experiment. Following this LDRD project, the PI was awarded a 5-year DOE early career research grant to further develop applications of laser-driven x-ray sources for high energy density science experiments and warm dense matter states.« less

Monitoring one-electron photo-oxidation of guanine in DNA crystals using ultrafast infrared spectroscopy.

PubMed

Hall, James P; Poynton, Fergus E; Keane, Páraic M; Gurung, Sarah P; Brazier, John A; Cardin, David J; Winter, Graeme; Gunnlaugsson, Thorfinnur; Sazanovich, Igor V; Towrie, Michael; Cardin, Christine J; Kelly, John M; Quinn, Susan J

2015-12-01

To understand the molecular origins of diseases caused by ultraviolet and visible light, and also to develop photodynamic therapy, it is important to resolve the mechanism of photoinduced DNA damage. Damage to DNA bound to a photosensitizer molecule frequently proceeds by one-electron photo-oxidation of guanine, but the precise dynamics of this process are sensitive to the location and the orientation of the photosensitizer, which are very difficult to define in solution. To overcome this, ultrafast time-resolved infrared (TRIR) spectroscopy was performed on photoexcited ruthenium polypyridyl-DNA crystals, the atomic structure of which was determined by X-ray crystallography. By combining the X-ray and TRIR data we are able to define both the geometry of the reaction site and the rates of individual steps in a reversible photoinduced electron-transfer process. This allows us to propose an individual guanine as the reaction site and, intriguingly, reveals that the dynamics in the crystal state are quite similar to those observed in the solvent medium.

Optical spectroscopy for food and beverages control

NASA Astrophysics Data System (ADS)

Mignani, Anna Grazia; Ciaccheri, Leonardo; Mencaglia, Andrea Azelio

2011-08-01

A selection of spectroscopy-based, fiber optic and micro-optic devices is presented. They have been designed and tested for monitoring the quality and safety of typical foodstuffs. The VIS-NIR spectra, considered as product fingerprints, allowed to discriminating the geographic region of production and to detecting nutritional and nutraceutic indicators.

Ultrafast carrier dynamics in the large-magnetoresistance material WTe 2

DOE PAGES

Dai, Y. M.; Bowlan, J.; Li, H.; ...

2015-10-07

In this study, ultrafast optical pump-probe spectroscopy is used to track carrier dynamics in the large-magnetoresistance material WTe 2. Our experiments reveal a fast relaxation process occurring on a subpicosecond time scale that is caused by electron-phonon thermalization, allowing us to extract the electron-phonon coupling constant. An additional slower relaxation process, occurring on a time scale of ~5–15 ps, is attributed to phonon-assisted electron-hole recombination. As the temperature decreases from 300 K, the time scale governing this process increases due to the reduction of the phonon population. However, below ~50 K, an unusual decrease of the recombination time sets in,more » most likely due to a change in the electronic structure that has been linked to the large magnetoresistance observed in this material.« less

Light-induced pyroelectric effect as an effective approach for ultrafast ultraviolet nanosensing

NASA Astrophysics Data System (ADS)

Wang, Zhaona; Yu, Ruomeng; Pan, Caofeng; Li, Zhaoling; Yang, Jin; Yi, Fang; Wang, Zhong Lin

2015-09-01

Zinc oxide is potentially a useful material for ultraviolet detectors; however, a relatively long response time hinders practical implementation. Here by designing and fabricating a self-powered ZnO/perovskite-heterostructured ultraviolet photodetector, the pyroelectric effect, induced in wurtzite ZnO nanowires on ultraviolet illumination, has been utilized as an effective approach for high-performance photon sensing. The response time is improved from 5.4 s to 53 μs at the rising edge, and 8.9 s to 63 μs at the falling edge, with an enhancement of five orders in magnitudes. The specific detectivity and the responsivity are both enhanced by 322%. This work provides a novel design to achieve ultrafast ultraviolet sensing at room temperature via light-self-induced pyroelectric effect. The newly designed ultrafast self-powered ultraviolet nanosensors may find promising applications in ultrafast optics, nonlinear optics, optothermal detections, computational memories and biocompatible optoelectronic probes.

Ultrafast Photo-Carrier Dynamics and Coherent Phonon Excitations in Topological Dirac Semimetal Cd3As2

NASA Astrophysics Data System (ADS)

Sun, Fei; Wu, Qiong; Wu, Yanling; Tian, Yichao; Shi, Youguo; Zhao, Jimin

Three dimensional (3D) topological Dirac semimetal has attracted growing research interest owing to its intriguing quantum properties such as high bulk carrier mobility and quantum spin Hall effects. However, so far, the ultrafast dynamics of a typical 3D topological Dirac semimetal, Cd3As2, as well as its coherent phonon has not been thoroughly investigated. Here we report the ultrafast dynamics of Cd3As2 by using femtosecond pump-probe spectroscopy. Two distinct relaxation processes was observed, with the lifetimes (at 5 K) of 2.4 ps and 18.6 ps, respectively. Variable temperature experiment from 5 K to 295 K also reveals signatures of phase transitions. Furthermore, coherent optical (8.1 meV) and acoustic (0.036 THz) phonon modes were generated and detected, respectively, with signatures of hybrid-excitation of the two modes. The National Basic Research Program of China (2012CB821402), the National Natural Science Foundation of China (11274372), and the External Cooperation Program of the Chinese Academy of Sciences (GJHZ1403).

Ultrafast optics. Ultrafast optical control by few photons in engineered fiber.

PubMed

Nissim, R; Pejkic, A; Myslivets, E; Kuo, B P; Alic, N; Radic, S

2014-07-25

Fast control of a strong optical beam by a few photons is an outstanding challenge that limits the performance of quantum sensors and optical processing devices. We report that a fast and efficient optical gate can be realized in an optical fiber that has been engineered with molecular-scale accuracy. Highly efficient, distributed phase-matched photon-photon interaction was achieved in the fiber with locally controlled, nanometer-scale core variations. A three-photon input was used to manipulate a Watt-scale beam at a speed exceeding 500 gigahertz. In addition to very fast beam control, the results provide a path to developing a new class of sensitive receivers capable of operating at very high rates. Copyright © 2014, American Association for the Advancement of Science.

Redox Conditions Affect Ultrafast Exciton Transport in Photosynthetic Pigment-Protein Complexes.

PubMed

Allodi, Marco A; Otto, John P; Sohail, Sara H; Saer, Rafael G; Wood, Ryan E; Rolczynski, Brian S; Massey, Sara C; Ting, Po-Chieh; Blankenship, Robert E; Engel, Gregory S

2018-01-04

Pigment-protein complexes in photosynthetic antennae can suffer oxidative damage from reactive oxygen species generated during solar light harvesting. How the redox environment of a pigment-protein complex affects energy transport on the ultrafast light-harvesting time scale remains poorly understood. Using two-dimensional electronic spectroscopy, we observe differences in femtosecond energy-transfer processes in the Fenna-Matthews-Olson (FMO) antenna complex under different redox conditions. We attribute these differences in the ultrafast dynamics to changes to the system-bath coupling around specific chromophores, and we identify a highly conserved tyrosine/tryptophan chain near the chromophores showing the largest changes. We discuss how the mechanism of tyrosine/tryptophan chain oxidation may contribute to these differences in ultrafast dynamics that can moderate energy transfer to downstream complexes where reactive oxygen species are formed. These results highlight the importance of redox conditions on the ultrafast transport of energy in photosynthesis. Tailoring the redox environment may enable energy transport engineering in synthetic light-harvesting systems.

Ultrafast Manipulation of Magnetic Order with Electrical Pulses

NASA Astrophysics Data System (ADS)

Yang, Yang

During the last 30 years spintronics has been a very rapidly expanding field leading to lots of new interesting physics and applications. As with most technology-oriented fields, spintronics strives to control devices with very low energy consumption and high speed. The combination of spin and electronics inherent to spintronics directly tackles energy efficiency, due to the non-volatility of magnetism. However, speed of operation of spintronic devices is still rather limited ( nanoseconds), due to slow magnetization precessional frequencies. Ultrafast magnetism (or opto-magnetism) is a relatively new field that has been very active in the last 20 years. The main idea is that intense femtosecond laser pulses can be used in order to manipulate the magnetization at very fast time-scales ( 100 femtoseconds). However, the use of femtosecond lasers poses great application challenges such as diffraction limited optical spot sizes which hinders device density, and bulky and expensive integration of femtosecond lasers into devices. In this thesis, our efforts to combine ultrafast magnetism and spintronics are presented. First, we show that the magnetization of ferrimagnetic GdFeCo films can be switched by picosecond electronic heat current pulses. This result shows that a non-thermal distribution of electrons directly excited by laser is not necessary for inducing ultrafast magnetic dynamics. Then, we fabricate photoconductive switch devices on a LT-GaAs substrate, to generate picosecond electrical pulses. Intense electrical pulses with 10ps (FWHM) duration and peak current up to 3A can be generated and delivered into magnetic films. Distinct magnetic dynamics in CoPt films are found between direct optical heating and electrical heating. More importantly, by delivering picosecond electrical pulses into GdFeCo films, we are able to deterministically reverse the magnetization of GdFeCo within 10ps. This is more than one order of magnitude faster than any other electrically

Ultrafast photoinduced charge separation in metal-semiconductor nanohybrids.

PubMed

Mongin, Denis; Shaviv, Ehud; Maioli, Paolo; Crut, Aurélien; Banin, Uri; Del Fatti, Natalia; Vallée, Fabrice

2012-08-28

Hybrid nano-objects formed by two or more disparate materials are among the most promising and versatile nanosystems. A key parameter in their properties is interaction between their components. In this context we have investigated ultrafast charge separation in semiconductor-metal nanohybrids using a model system of gold-tipped CdS nanorods in a matchstick architecture. Experiments are performed using an optical time-resolved pump-probe technique, exciting either the semiconductor or the metal component of the particles, and probing the light-induced change of their optical response. Electron-hole pairs photoexcited in the semiconductor part of the nanohybrids are shown to undergo rapid charge separation with the electron transferred to the metal part on a sub-20 fs time scale. This ultrafast gold charging leads to a transient red-shift and broadening of the metal surface plasmon resonance, in agreement with results for free clusters but in contrast to observation for static charging of gold nanoparticles in liquid environments. Quantitative comparison with a theoretical model is in excellent agreement with the experimental results, confirming photoexcitation of one electron-hole pair per nanohybrid followed by ultrafast charge separation. The results also point to the utilization of such metal-semiconductor nanohybrids in light-harvesting applications and in photocatalysis.

Ultrafast kinetics of linkage isomerism in Na2[Fe(CN)5NO] aqueous solution revealed by time-resolved photoelectron spectroscopy

PubMed Central

Raheem, Azhr A.; Wilke, Martin; Borgwardt, Mario; Engel, Nicholas; Bokarev, Sergey I.; Grell, Gilbert; Aziz, Saadullah G.; Kühn, Oliver; Kiyan, Igor Yu.; Merschjann, Christoph; Aziz, Emad F.

2017-01-01

The kinetics of ultrafast photoinduced structural changes in linkage isomers is investigated using Na2[Fe(CN)5NO] as a model complex. The buildup of the metastable side-on configuration of the NO ligand, as well as the electronic energy levels of ground, excited, and metastable states, has been revealed by means of time-resolved extreme UV (XUV) photoelectron spectroscopy in aqueous solution, aided by theoretical calculations. Evidence of a short-lived intermediate state in the isomerization process and its nature are discussed, finding that the complete isomerization process occurs in less than 240 fs after photoexcitation. PMID:28713840

Probing ultrafast proton induced dynamics in transparent dielectrics

NASA Astrophysics Data System (ADS)

Taylor, M.; Coughlan, M.; Nersisyan, G.; Senje, L.; Jung, D.; Currell, F.; Riley, D.; Lewis, C. L. S.; Zepf, M.; Dromey, B.

2018-05-01

A scheme has been developed permitting the spatial and temporal characterisation of ultrafast dynamics induced by laser driven proton bursts in transparent dielectrics. Advantage is taken of the high degree of synchronicity between the proton bursts generated during laser-foil target interactions and the probing laser to provide the basis for streaking of the dynamics. Relaxation times of electrons (<10‑12 s) are measured following swift excitation across the optical band gap for various glass samples. A temporal resolution of <500 fs is achieved demonstrating that these ultrafast dynamics can be characterized on a single-shot basis.

Polarization and Thickness Dependent Absorption Properties of Black Phosphorus: New Saturable Absorber for Ultrafast Pulse Generation

PubMed Central

Li, Diao; Jussila, Henri; Karvonen, Lasse; Ye, Guojun; Lipsanen, Harri; Chen, Xianhui; Sun, Zhipei

2015-01-01

Black phosphorus (BP) has recently been rediscovered as a new and interesting two-dimensional material due to its unique electronic and optical properties. Here, we study the linear and nonlinear optical properties of BP flakes. We observe that both the linear and nonlinear optical properties are anisotropic and can be tuned by the film thickness in BP, completely different from other typical two-dimensional layered materials (e.g., graphene and the most studied transition metal dichalcogenides). We then use the nonlinear optical properties of BP for ultrafast (pulse duration down to ~786 fs in mode-locking) and large-energy (pulse energy up to >18 nJ in Q-switching) pulse generation in fiber lasers at the near-infrared telecommunication band ~1.5 μm. We observe that the output of our BP based pulsed lasers is linearly polarized (with a degree-of-polarization ~98% in mode-locking, >99% in Q-switching, respectively) due to the anisotropic optical property of BP. Our results underscore the relatively large optical nonlinearity of BP with unique polarization and thickness dependence, and its potential for polarized optical pulse generation, paving the way to BP based nonlinear and ultrafast photonic applications (e.g., ultrafast all-optical polarization switches/modulators, frequency converters etc.). PMID:26514090

Cross-phase modulation bandwidth in ultrafast fiber wavelength converters

NASA Astrophysics Data System (ADS)

Luís, Ruben S.; Monteiro, Paulo; Teixeira, António

2006-12-01

We propose a novel analytical model for the characterization of fiber cross-phase modulation (XPM) in ultrafast all-optical fiber wavelength converters, operating at modulation frequencies higher than 1THz. The model is used to compare the XPM frequency limitations of a conventional and a highly nonlinear dispersion shifted fiber (HN-DSF) and a bismuth oxide-based fiber, introducing the XPM bandwidth as a design parameter. It is shown that the HN-DSF presents the highest XPM bandwidth, above 1THz, making it the most appropriate for ultrafast wavelength conversion.

Complete quantum control of a single quantum dot spin using ultrafast optical pulses.

PubMed

Press, David; Ladd, Thaddeus D; Zhang, Bingyang; Yamamoto, Yoshihisa

2008-11-13

A basic requirement for quantum information processing systems is the ability to completely control the state of a single qubit. For qubits based on electron spin, a universal single-qubit gate is realized by a rotation of the spin by any angle about an arbitrary axis. Driven, coherent Rabi oscillations between two spin states can be used to demonstrate control of the rotation angle. Ramsey interference, produced by two coherent spin rotations separated by a variable time delay, demonstrates control over the axis of rotation. Full quantum control of an electron spin in a quantum dot has previously been demonstrated using resonant radio-frequency pulses that require many spin precession periods. However, optical manipulation of the spin allows quantum control on a picosecond or femtosecond timescale, permitting an arbitrary rotation to be completed within one spin precession period. Recent work in optical single-spin control has demonstrated the initialization of a spin state in a quantum dot, as well as the ultrafast manipulation of coherence in a largely unpolarized single-spin state. Here we demonstrate complete coherent control over an initialized electron spin state in a quantum dot using picosecond optical pulses. First we vary the intensity of a single optical pulse to observe over six Rabi oscillations between the two spin states; then we apply two sequential pulses to observe high-contrast Ramsey interference. Such a two-pulse sequence realizes an arbitrary single-qubit gate completed on a picosecond timescale. Along with the spin initialization and final projective measurement of the spin state, these results demonstrate a complete set of all-optical single-qubit operations.

Layer-Dependent Ultrafast Carrier and Coherent Phonon Dynamics in Black Phosphorus.

PubMed

Miao, Xianchong; Zhang, Guowei; Wang, Fanjie; Yan, Hugen; Ji, Minbiao

2018-05-09

Black phosphorus is a layered semiconducting material, demonstrating strong layer-dependent optical and electronic properties. Probing the photophysical properties on ultrafast time scales is of central importance in understanding many-body interactions and nonequilibrium quasiparticle dynamics. Here, we applied temporally, spectrally, and spatially resolved pump-probe microscopy to study the transient optical responses of mechanically exfoliated few-layer black phosphorus, with layer numbers ranging from 2 to 9. We have observed layer-dependent resonant transient absorption spectra with both photobleaching and red-shifted photoinduced absorption features, which could be attributed to band gap renormalization of higher subband transitions. Surprisingly, coherent phonon oscillations with unprecedented intensities were observed when the probe photons were in resonance with the optical transitions, which correspond to the low-frequency layer-breathing mode. Our results reveal strong Coulomb interactions and electron-phonon couplings in photoexcited black phosphorus, providing important insights into the ultrafast optical, nanomechanical, and optoelectronic properties of this novel two-dimensional material.

Tuning ultrafast electron injection dynamics at organic-graphene/metal interfaces.

PubMed

Ravikumar, Abhilash; Kladnik, Gregor; Müller, Moritz; Cossaro, Albano; Bavdek, Gregor; Patera, Laerte L; Sánchez-Portal, Daniel; Venkataraman, Latha; Morgante, Alberto; Brivio, Gian Paolo; Cvetko, Dean; Fratesi, Guido

2018-05-03

We compare the ultrafast charge transfer dynamics of molecules on epitaxial graphene and bilayer graphene grown on Ni(111) interfaces through first principles calculations and X-ray resonant photoemission spectroscopy. We use 4,4'-bipyridine as a prototypical molecule for these explorations as the energy level alignment of core-excited molecular orbitals allows ultrafast injection of electrons from a substrate to a molecule on a femtosecond timescale. We show that the ultrafast injection of electrons from the substrate to the molecule is ∼4 times slower on weakly coupled bilayer graphene than on epitaxial graphene. Through our experiments and calculations, we can attribute this to a difference in the density of states close to the Fermi level between graphene and bilayer graphene. We therefore show how graphene coupling with the substrate influences charge transfer dynamics between organic molecules and graphene interfaces.

Effect of additional optical pumping injection into the ground-state ensemble on the gain and the phase recovery acceleration of quantum-dot semiconductor optical amplifiers

NASA Astrophysics Data System (ADS)

Kim, Jungho

2014-02-01

The effect of additional optical pumping injection into the ground-state ensemble on the ultrafast gain and the phase recovery dynamics of electrically-driven quantum-dot semiconductor optical amplifiers is numerically investigated by solving 1088 coupled rate equations. The ultrafast gain and the phase recovery responses are calculated with respect to the additional optical pumping power. Increasing the additional optical pumping power can significantly accelerate the ultrafast phase recovery, which cannot be done by increasing the injection current density.

Single-shot Monitoring of Ultrafast Processes via X-ray Streaking at a Free Electron Laser.

PubMed

Buzzi, Michele; Makita, Mikako; Howald, Ludovic; Kleibert, Armin; Vodungbo, Boris; Maldonado, Pablo; Raabe, Jörg; Jaouen, Nicolas; Redlin, Harald; Tiedtke, Kai; Oppeneer, Peter M; David, Christian; Nolting, Frithjof; Lüning, Jan

2017-08-03

The advent of x-ray free electron lasers has extended the unique capabilities of resonant x-ray spectroscopy techniques to ultrafast time scales. Here, we report on a novel experimental method that allows retrieving with a single x-ray pulse the time evolution of an ultrafast process, not only at a few discrete time delays, but continuously over an extended time window. We used a single x-ray pulse to resolve the laser-induced ultrafast demagnetisation dynamics in a thin cobalt film over a time window of about 1.6 ps with an excellent signal to noise ratio. From one representative single shot measurement we extract a spin relaxation time of (130 ± 30) fs with an average value, based on 193 single shot events of (113 ± 20) fs. These results are limited by the achieved experimental time resolution of 120 fs, and both values are in excellent agreement with previous results and theoretical modelling. More generally, this new experimental approach to ultrafast x-ray spectroscopy paves the way to the study of non-repetitive processes that cannot be investigated using traditional repetitive pump-probe schemes.

Ultrafast carrier thermalization and trapping in silicon-germanium alloy probed by extreme ultraviolet transient absorption spectroscopy

DOE PAGES

Zürch, Michael; Chang, Hung-Tzu; Kraus, Peter M.; ...

2017-06-06

Semiconductor alloys containing silicon and germanium are of growing importance for compact and highly efficient photonic devices due to their favorable properties for direct integration into silicon platforms and wide tunability of optical parameters. Here, we report the simultaneous direct and energy-resolved probing of ultrafast electron and hole dynamics in a silicon-germanium alloy with the stoichiometry Si 0.25Ge 0.75 by extreme ultraviolet transient absorption spectroscopy. Probing the photoinduced dynamics of charge carriers at the germanium M 4,5-edge (~30 eV) allows the germanium atoms to be used as reporter atoms for carrier dynamics in the alloy. The photoexcitation of electrons acrossmore » the direct and indirect band gap into conduction band (CB) valleys and their subsequent hot carrier relaxation are observed and compared to pure germanium, where the Ge direct (ΔE gap,Ge,direct = 0.8 eV) and Si 0.25Ge 0.75 indirect gaps (ΔE gap,Si0.25Ge0.75,indirect = 0.95 eV) are comparable in energy. In the alloy, comparable carrier lifetimes are observed for the X, L, and Γ valleys in the conduction band. A midgap feature associated with electrons accumulating in trap states near the CB edge following intraband thermalization is observed in the Si 0.25Ge 0.75 alloy. The successful implementation of the reporter atom concept for capturing the dynamics of the electronic bands by site-specific probing in solids opens a route to study carrier dynamics in more complex materials with femtosecond and sub-femtosecond temporal resolution.« less

Ultrafast carrier thermalization and trapping in silicon-germanium alloy probed by extreme ultraviolet transient absorption spectroscopy

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

Zürch, Michael; Chang, Hung-Tzu; Kraus, Peter M.

Semiconductor alloys containing silicon and germanium are of growing importance for compact and highly efficient photonic devices due to their favorable properties for direct integration into silicon platforms and wide tunability of optical parameters. Here, we report the simultaneous direct and energy-resolved probing of ultrafast electron and hole dynamics in a silicon-germanium alloy with the stoichiometry Si 0.25Ge 0.75 by extreme ultraviolet transient absorption spectroscopy. Probing the photoinduced dynamics of charge carriers at the germanium M 4,5-edge (~30 eV) allows the germanium atoms to be used as reporter atoms for carrier dynamics in the alloy. The photoexcitation of electrons acrossmore » the direct and indirect band gap into conduction band (CB) valleys and their subsequent hot carrier relaxation are observed and compared to pure germanium, where the Ge direct (ΔE gap,Ge,direct = 0.8 eV) and Si 0.25Ge 0.75 indirect gaps (ΔE gap,Si0.25Ge0.75,indirect = 0.95 eV) are comparable in energy. In the alloy, comparable carrier lifetimes are observed for the X, L, and Γ valleys in the conduction band. A midgap feature associated with electrons accumulating in trap states near the CB edge following intraband thermalization is observed in the Si 0.25Ge 0.75 alloy. The successful implementation of the reporter atom concept for capturing the dynamics of the electronic bands by site-specific probing in solids opens a route to study carrier dynamics in more complex materials with femtosecond and sub-femtosecond temporal resolution.« less

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.

Optical spectroscopies diagnose cancer

NASA Astrophysics Data System (ADS)

Alfano, Robert R.; Das, Bidyut B.; Glassman, Wenling S.; Pradhan, Asima; Tang, Gui C.

1992-02-01

Today's medical professional is looking beyond the conventional procedures of X-rays, nuclear radiation, magnetic resonance, chemical analysis, and ultrasound to diagnose diseases ranging from cancer to heart ailments. In view of the possible dangerous side effects of X-rays and nuclear radiation, a need exists for novel techniques in disease detection that can either eliminate or reduce their use in examinations. For more than half a century, fluorescence, absorption, and light scattering spectroscopies have been widely used as probes to acquire fundamental knowledge about various physical, chemical, and biological processes. Light may offer alternatives to X-rays and nuclear approaches, and in some cases is non-invasive. Optical spectroscopy and laser technology may offer techniques for the detection and characterization of physical and chemical changes that occur in diseased tissue on a microscopic level.

Ultrafast Transient Absorption Spectroscopy Investigation of Photoinduced Dynamics in Novel Donor-Acceptor Core-Shell Nanostructures for Organic Photovoltaics

NASA Astrophysics Data System (ADS)

Strain, Jacob; Jamhawi, Abdelqader; Abeywickrama, Thulitha M.; Loomis, Wendy; Rathnayake, Hemali; Liu, Jinjun

2016-06-01

Novel donor-acceptor nanostructures were synthesized via covalent synthesis and/or UV cross-linking method. Their photoinduced dynamics were investigated with ultrafast transient absorption (TA) spectroscopy. These new nanostructures are made with the strategy in mind to reduce manufacturing steps in the process of fabricating an organic photovoltaic cell. By imitating the heterojunction interface within a fixed particle domain, several fabrication steps can be bypassed reducing cost and giving more applicability to other film deposition methods. Such applications include aerosol deposition and ink-jet printing. The systems that were studied by TA spectroscopy include PDIB core, PDIB-P3HT core-shell, and PDIB-PANT core-shell which range in size from 60 to 130 nm. Within the experimentally accessible spectra range there resides a region of ground state bleaching, stimulated emission, and excited-state absorption of both neutrals and anions. Control experiments have been carried out to assign these features. At high pump fluences the TA spectra of PDIB core alone also indicate an intramolecular charge separation. The TA spectroscopy results thus far suggest that the core-shells resemble the photoinduced dynamics of a standard film although the particles are dispersed in solution, which indicates the desired outcome of the work.

Ultrafast photocurrents in monolayer MoS2

NASA Astrophysics Data System (ADS)

Parzinger, Eric; Wurstbauer, Ursula; Holleitner, Alexander W.

Two-dimensional transition metal dichalcogenides such as MoS2 have emerged as interesting materials for optoelectronic devices. In particular, the ultrafast dynamics and lifetimes of photoexcited charge carriers have attracted great interest during the last years. We investigate the photocurrent response of monolayer MoS2 on a picosecond time scale utilizing a recently developed pump-probe spectroscopy technique based on coplanar striplines. We discuss the ultrafast dynamics within MoS2 including photo-thermoelectric currents and the impact of built-in fields due to Schottky barriers as well as the Fermi level pinning at the contact region. We acknowledge support by the ERC via Project 'NanoREAL', the DFG via excellence cluster 'Nanosystems Initiative Munich' (NIM), and through the TUM International Graduate School of Science and Engineering (IGSSE) and BaCaTeC.

Perspective: Ultrafast magnetism and THz spintronics

NASA Astrophysics Data System (ADS)

Walowski, Jakob; Münzenberg, Markus

2016-10-01

This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time, this milestone work by Bigot and coworkers gave insight directly into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than providing an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledge the first applications are developed: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. Based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address the processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first usage of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.

Perspective: Ultrafast magnetism and THz spintronics

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

Walowski, Jakob; Münzenberg, Markus

This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time, this milestone work by Bigot and coworkers gave insight directly into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than providing an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledgemore » the first applications are developed: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. Based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address the processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first usage of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.« less

Thermal effects in an ultrafast BiB 3O 6 optical parametric oscillator at high average powers

DOE PAGES

Petersen, T.; Zuegel, J. D.; Bromage, J.

2017-08-15

An ultrafast, high-average-power, extended-cavity, femtosecond BiB 3O 6 optical parametric oscillator was constructed as a test bed for investigating the scalability of infrared parametric devices. Despite the high pulse energies achieved by this system, the reduction in slope efficiency near the maximum-available pump power prompted the investigation of thermal effects in the crystal during operation. Furthermore, the local heating effects in the crystal were used to determine the impact on both phase matching and thermal lensing to understand limitations that must be overcome to achieve microjoule-level pulse energies at high repetition rates.

Thermal effects in an ultrafast BiB 3O 6 optical parametric oscillator at high average powers

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

Petersen, T.; Zuegel, J. D.; Bromage, J.

An ultrafast, high-average-power, extended-cavity, femtosecond BiB 3O 6 optical parametric oscillator was constructed as a test bed for investigating the scalability of infrared parametric devices. Despite the high pulse energies achieved by this system, the reduction in slope efficiency near the maximum-available pump power prompted the investigation of thermal effects in the crystal during operation. Furthermore, the local heating effects in the crystal were used to determine the impact on both phase matching and thermal lensing to understand limitations that must be overcome to achieve microjoule-level pulse energies at high repetition rates.

Nanoscale diffractive probing of strain dynamics in ultrafast transmission electron microscopy

PubMed Central

Feist, Armin; Rubiano da Silva, Nara; Liang, Wenxi; Ropers, Claus; Schäfer, Sascha

2018-01-01

The control of optically driven high-frequency strain waves in nanostructured systems is an essential ingredient for the further development of nanophononics. However, broadly applicable experimental means to quantitatively map such structural distortion on their intrinsic ultrafast time and nanometer length scales are still lacking. Here, we introduce ultrafast convergent beam electron diffraction with a nanoscale probe beam for the quantitative retrieval of the time-dependent local deformation gradient tensor. We demonstrate its capabilities by investigating the ultrafast acoustic deformations close to the edge of a single-crystalline graphite membrane. Tracking the structural distortion with a 28-nm/700-fs spatio-temporal resolution, we observe an acoustic membrane breathing mode with spatially modulated amplitude, governed by the optical near field structure at the membrane edge. Furthermore, an in-plane polarized acoustic shock wave is launched at the membrane edge, which triggers secondary acoustic shear waves with a pronounced spatio-temporal dependency. The experimental findings are compared to numerical acoustic wave simulations in the continuous medium limit, highlighting the importance of microscopic dissipation mechanisms and ballistic transport channels. PMID:29464187

Nanoscale diffractive probing of strain dynamics in ultrafast transmission electron microscopy.

PubMed

Feist, Armin; Rubiano da Silva, Nara; Liang, Wenxi; Ropers, Claus; Schäfer, Sascha

2018-01-01

The control of optically driven high-frequency strain waves in nanostructured systems is an essential ingredient for the further development of nanophononics. However, broadly applicable experimental means to quantitatively map such structural distortion on their intrinsic ultrafast time and nanometer length scales are still lacking. Here, we introduce ultrafast convergent beam electron diffraction with a nanoscale probe beam for the quantitative retrieval of the time-dependent local deformation gradient tensor. We demonstrate its capabilities by investigating the ultrafast acoustic deformations close to the edge of a single-crystalline graphite membrane. Tracking the structural distortion with a 28-nm/700-fs spatio-temporal resolution, we observe an acoustic membrane breathing mode with spatially modulated amplitude, governed by the optical near field structure at the membrane edge. Furthermore, an in-plane polarized acoustic shock wave is launched at the membrane edge, which triggers secondary acoustic shear waves with a pronounced spatio-temporal dependency. The experimental findings are compared to numerical acoustic wave simulations in the continuous medium limit, highlighting the importance of microscopic dissipation mechanisms and ballistic transport channels.

Ultrafast ultrasound localization microscopy for deep super-resolution vascular imaging

NASA Astrophysics Data System (ADS)

Errico, Claudia; Pierre, Juliette; Pezet, Sophie; Desailly, Yann; Lenkei, Zsolt; Couture, Olivier; Tanter, Mickael

2015-11-01

Non-invasive imaging deep into organs at microscopic scales remains an open quest in biomedical imaging. Although optical microscopy is still limited to surface imaging owing to optical wave diffusion and fast decorrelation in tissue, revolutionary approaches such as fluorescence photo-activated localization microscopy led to a striking increase in resolution by more than an order of magnitude in the last decade. In contrast with optics, ultrasonic waves propagate deep into organs without losing their coherence and are much less affected by in vivo decorrelation processes. However, their resolution is impeded by the fundamental limits of diffraction, which impose a long-standing trade-off between resolution and penetration. This limits clinical and preclinical ultrasound imaging to a sub-millimetre scale. Here we demonstrate in vivo that ultrasound imaging at ultrafast frame rates (more than 500 frames per second) provides an analogue to optical localization microscopy by capturing the transient signal decorrelation of contrast agents—inert gas microbubbles. Ultrafast ultrasound localization microscopy allowed both non-invasive sub-wavelength structural imaging and haemodynamic quantification of rodent cerebral microvessels (less than ten micrometres in diameter) more than ten millimetres below the tissue surface, leading to transcranial whole-brain imaging within short acquisition times (tens of seconds). After intravenous injection, single echoes from individual microbubbles were detected through ultrafast imaging. Their localization, not limited by diffraction, was accumulated over 75,000 images, yielding 1,000,000 events per coronal plane and statistically independent pixels of ten micrometres in size. Precise temporal tracking of microbubble positions allowed us to extract accurately in-plane velocities of the blood flow with a large dynamic range (from one millimetre per second to several centimetres per second). These results pave the way for deep non

Ultrafast ultrasound localization microscopy for deep super-resolution vascular imaging.

PubMed

Errico, Claudia; Pierre, Juliette; Pezet, Sophie; Desailly, Yann; Lenkei, Zsolt; Couture, Olivier; Tanter, Mickael

2015-11-26

Non-invasive imaging deep into organs at microscopic scales remains an open quest in biomedical imaging. Although optical microscopy is still limited to surface imaging owing to optical wave diffusion and fast decorrelation in tissue, revolutionary approaches such as fluorescence photo-activated localization microscopy led to a striking increase in resolution by more than an order of magnitude in the last decade. In contrast with optics, ultrasonic waves propagate deep into organs without losing their coherence and are much less affected by in vivo decorrelation processes. However, their resolution is impeded by the fundamental limits of diffraction, which impose a long-standing trade-off between resolution and penetration. This limits clinical and preclinical ultrasound imaging to a sub-millimetre scale. Here we demonstrate in vivo that ultrasound imaging at ultrafast frame rates (more than 500 frames per second) provides an analogue to optical localization microscopy by capturing the transient signal decorrelation of contrast agents--inert gas microbubbles. Ultrafast ultrasound localization microscopy allowed both non-invasive sub-wavelength structural imaging and haemodynamic quantification of rodent cerebral microvessels (less than ten micrometres in diameter) more than ten millimetres below the tissue surface, leading to transcranial whole-brain imaging within short acquisition times (tens of seconds). After intravenous injection, single echoes from individual microbubbles were detected through ultrafast imaging. Their localization, not limited by diffraction, was accumulated over 75,000 images, yielding 1,000,000 events per coronal plane and statistically independent pixels of ten micrometres in size. Precise temporal tracking of microbubble positions allowed us to extract accurately in-plane velocities of the blood flow with a large dynamic range (from one millimetre per second to several centimetres per second). These results pave the way for deep non

A novel solid solution LiGa(S1–x Se x )2 for generating coherent ultrafast mid-IR sources

NASA Astrophysics Data System (ADS)

Jer Huang, Jin; Zhang, Xin Lu; Feng, Qian; Dai, Jun Feng; Andreev, Yury M.; Lanskii, Grigory V.; Grechin, Sergei G.

2018-06-01

With renewed refractive indices, the potential of a solid solution () in optical frequency conversion—especially in phase matching and group velocity matching—is theoretically investigated, together with the composition ratio limitation. It is found that the solution has excellent features for generating coherent ultrafast mid-IR sources covering 8–11 μm, which can be realized by type II down-conversion in the ba-plane with perfect group velocity matching, or type I in the bc-plane with part group velocity matching. This will have broad applications in LiDAR monitoring and precision spectroscopy, as well as life and environmental sciences.

Dynamics of Functionalized Surface Molecular Monolayers Studied with Ultrafast Infrared Vibrational Spectroscopy

PubMed Central

Rosenfeld, Daniel E.; Nishida, Jun; Yan, Chang; Gengeliczki, Zsolt; Smith, Brian J.; Fayer, Michael D.

2012-01-01

The structural dynamics of thin films consisting of tricarbonyl (1,10-phenanthroline)rhenium chloride (RePhen(CO)3Cl) linked to an alkyl silane monolayer through a triazole linker synthesized on silica-on-calcium-fluoride substrates are investigated using ultrafast infrared (IR) techniques. Ultrafast 2D IR vibrational echo experiments and polarization selective heterodyne detected transient grating (HDTG) measurements, as well as polarization dependent FT-IR and AFM experiments are employed to study the samples. The vibrational echo experiments measure spectral diffusion, while the HDTG experiments measure the vibrational excited state population relaxation and investigate the vibrational transition dipole orientational anisotropy decay. To investigate the anticipated impact of vibrational excitation transfer, which can be caused by the high concentration of RePhen(CO)3Cl in the monolayer, a concentration dependence of the spectral diffusion is measured. To generate a range of concentrations, mixed monolayers consisting of both hydrogen terminated and triazole/RePhen(CO)3Cl terminated alkyl silanes are synthesized. It is found that the measured rate of spectral diffusion is independent of concentration, with all samples showing spectral diffusion of 37 ± 6 ps. To definitively test for vibrational excitation transfer, polarization selective HDTG experiments are conducted. Excitation transfer will cause anisotropy decay. Polarization resolved heterodyne detected transient grating spectroscopy is sensitive to anisotropy decay (depolarization) caused by excitation transfer and molecular reorientation. The HDTG experiments show no evidence of anisotropy decay on the appropriate time scale, demonstrating the absence of excitation transfer the RePhen(CO)3Cl. Therefore the influence of excitation transfer on spectral diffusion is inconsequential in these samples, and the vibrational echo measurements of spectral diffusion report solely on structural dynamics. A small

Method and apparatus for two-dimensional spectroscopy

DOEpatents

DeCamp, Matthew F.; Tokmakoff, Andrei

2010-10-12

Preferred embodiments of the invention provide for methods and systems of 2D spectroscopy using ultrafast, first light and second light beams and a CCD array detector. A cylindrically-focused second light beam interrogates a target that is optically interactive with a frequency-dispersed excitation (first light) pulse, whereupon the second light beam is frequency-dispersed at right angle orientation to its line of focus, so that the horizontal dimension encodes the spatial location of the second light pulse and the first light frequency, while the vertical dimension encodes the second light frequency. Differential spectra of the first and second light pulses result in a 2D frequency-frequency surface equivalent to double-resonance spectroscopy. Because the first light frequency is spatially encoded in the sample, an entire surface can be acquired in a single interaction of the first and second light pulses.

Indirect excitation of ultrafast demagnetization

DOE PAGES

Vodungbo, Boris; Tudu, Bahrati; Perron, Jonathan; ...

2016-01-06

Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset andmore » at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. As a result, our data thus confirm recent theoretical predictions.« less

Indirect excitation of ultrafast demagnetization

PubMed Central

Vodungbo, Boris; Tudu, Bahrati; Perron, Jonathan; Delaunay, Renaud; Müller, Leonard; Berntsen, Magnus H.; Grübel, Gerhard; Malinowski, Grégory; Weier, Christian; Gautier, Julien; Lambert, Guillaume; Zeitoun, Philippe; Gutt, Christian; Jal, Emmanuelle; Reid, Alexander H.; Granitzka, Patrick W.; Jaouen, Nicolas; Dakovski, Georgi L.; Moeller, Stefan; Minitti, Michael P.; Mitra, Ankush; Carron, Sebastian; Pfau, Bastian; von Korff Schmising, Clemens; Schneider, Michael; Eisebitt, Stefan; Lüning, Jan

2016-01-01

Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions. PMID:26733106

Ultrafast all-optical flip-flop based on passive micro Sagnac waveguide ring with photonic crystal fiber.

PubMed

Xu, Ming; Yang, Wan; Hong, Tao; Kang, TangZhen; Ji, JianHua; Wang, Ke

2017-06-01

Ultrafast all-optical flip-flop based on a passive micro Sagnac waveguide ring is studied through theoretical analysis and numerical simulation in this paper. The types of D, R-S, J-K, and T flip-flop are designed by controlling the cross-phase modulation effect of lights in this special microring. The high nonlinearity of the hollow-core photonic crystal fiber is implanted on a chip to shorten the length of the ring and reduce input power. By sensible management, the pulse width ratio of the input and the control signal, problems of pulse narrowing, and residual pedestal at the out port are solved. The parameters affecting the performance of flip-flops are optimized. The results show that the all-optical flip-flops have stable performance, low power consumption, high transmission rate (up to 100  Gb/s), and response time in picosecond order. The small size microwaveguide structure is suitable for photonic integration.

Optical spectroscopy of laser-produced plasmas for standoff isotopic analysis

NASA Astrophysics Data System (ADS)

Harilal, S. S.; Brumfield, B. E.; LaHaye, N. L.; Hartig, K. C.; Phillips, M. C.

2018-06-01

Rapid, in-field, and non-contact isotopic analysis of solid materials is extremely important to a large number of applications, such as nuclear nonproliferation monitoring and forensics, geochemistry, archaeology, and biochemistry. Presently, isotopic measurements for these and many other fields are performed in laboratory settings. Rapid, in-field, and non-contact isotopic analysis of solid material is possible with optical spectroscopy tools when combined with laser ablation. Laser ablation generates a transient vapor of any solid material when a powerful laser interacts with a sample of interest. Analysis of atoms, ions, and molecules in a laser-produced plasma using optical spectroscopy tools can provide isotopic information with the advantages of real-time analysis, standoff capability, and no sample preparation requirement. Both emission and absorption spectroscopy methods can be used for isotopic analysis of solid materials. However, applying optical spectroscopy to the measurement of isotope ratios from solid materials presents numerous challenges. Isotope shifts arise primarily due to variation in nuclear charge distribution caused by different numbers of neutrons, but the small proportional nuclear mass differences between nuclei of various isotopes lead to correspondingly small differences in optical transition wavelengths. Along with this, various line broadening mechanisms in laser-produced plasmas and instrumental broadening generated by the detection system are technical challenges frequently encountered with emission-based optical diagnostics. These challenges can be overcome by measuring the isotope shifts associated with the vibronic emission bands from molecules or by using the techniques of laser-based absorption/fluorescence spectroscopy to marginalize the effect of instrumental broadening. Absorption and fluorescence spectroscopy probe the ground state atoms existing in the plasma when it is cooler, which inherently provides narrower

Enhanced Ultrafast Nonlinear Optics With Microstructure Fibers And Photonic Crystals

DTIC Science & Technology

2004-07-01

NANOHOLES FREQUENCY-TUNABLE ANTI-STOKES LINE EMISSION BY EIGENMODES OF A BIREFRINGENT MICROSTRUCTURE FIBER GENERATION OF FEMTOSECOND ANTI-STOKES PULSES...laser technologies, and ultrafast photonics. ANTI-STOKES GENERATION IN GUIDED MODES OF PHOTONIC-CRYSTAL FIBERS MODIFIED WITH AN ARRAY OF NANOHOLES

High-speed ultrafast laser machining with tertiary beam positioning (Conference Presentation)

NASA Astrophysics Data System (ADS)

Yang, Chuan; Zhang, Haibin

2017-03-01

For an industrial laser application, high process throughput and low average cost of ownership are critical to commercial success. Benefiting from high peak power, nonlinear absorption and small-achievable spot size, ultrafast lasers offer advantages of minimal heat affected zone, great taper and sidewall quality, and small via capability that exceeds the limits of their predecessors in via drilling for electronic packaging. In the past decade, ultrafast lasers have both grown in power and reduced in cost. For example, recently, disk and fiber technology have both shown stable operation in the 50W to 200W range, mostly at high repetition rate (beyond 500 kHz) that helps avoid detrimental nonlinear effects. However, to effectively and efficiently scale the throughput with the fast-growing power capability of the ultrafast lasers while keeping the beneficial laser-material interactions is very challenging, mainly because of the bottleneck imposed by the inertia-related acceleration limit and servo gain bandwidth when only stages and galvanometers are being used. On the other side, inertia-free scanning solutions like acoustic optics and electronic optical deflectors have small scan field, and therefore not suitable for large-panel processing. Our recent system developments combine stages, galvanometers, and AODs into a coordinated tertiary architecture for high bandwidth and meanwhile large field beam positioning. Synchronized three-level movements allow extremely fast local speed and continuous motion over the whole stage travel range. We present the via drilling results from such ultrafast system with up to 3MHz pulse to pulse random access, enabling high quality low cost ultrafast machining with emerging high average power laser sources.

Ultrafast laser processing of copper: A comparative study of experimental and simulated transient optical properties

NASA Astrophysics Data System (ADS)

Winter, Jan; Rapp, Stephan; Schmidt, Michael; Huber, Heinz P.

2017-09-01

In this paper, we present ultrafast measurements of the complex refractive index for copper up to a time delay of 20 ps with an accuracy <1% at laser fluences in the vicinity of the ablation threshold. The measured refractive index n and extinction coefficient k are supported by a simulation including the two-temperature model with an accurate description of thermal and optical properties and a thermomechanical model. Comparison of the measured time resolved optical properties with results of the simulation reveals underlying physical mechanisms in three distinct time delay regimes. It is found that in the early stage (-5 ps to 0 ps) the thermally excited d-band electrons make a major contribution to the laser pulse absorption and create a steep increase in transient optical properties n and k. In the second time regime (0-10 ps) the material expansion influences the plasma frequency, which is also reflected in the transient extinction coefficient. In contrast, the refractive index n follows the total collision frequency. Additionally, the electron-ion thermalization time can be attributed to a minimum of the extinction coefficient at ∼10 ps. In the third time regime (10-20 ps) the transient extinction coefficient k indicates the surface cooling-down process.

Selective ultrafast probing of transient hot chemisorbed and precursor states of CO on Ru(0001).

PubMed

Beye, M; Anniyev, T; Coffee, R; Dell'Angela, M; Föhlisch, A; Gladh, J; Katayama, T; Kaya, S; Krupin, O; Møgelhøj, A; Nilsson, A; Nordlund, D; Nørskov, J K; Öberg, H; Ogasawara, H; Pettersson, L G M; Schlotter, W F; Sellberg, J A; Sorgenfrei, F; Turner, J J; Wolf, M; Wurth, W; Oström, H

2013-05-03

We have studied the femtosecond dynamics following optical laser excitation of CO adsorbed on a Ru surface by monitoring changes in the occupied and unoccupied electronic structure using ultrafast soft x-ray absorption and emission. We recently reported [M. Dell'Angela et al. Science 339, 1302 (2013)] a phonon-mediated transition into a weakly adsorbed precursor state occurring on a time scale of >2 ps prior to desorption. Here we focus on processes within the first picosecond after laser excitation and show that the metal-adsorbate coordination is initially increased due to hot-electron-driven vibrational excitations. This process is faster than, but occurs in parallel with, the transition into the precursor state. With resonant x-ray emission spectroscopy, we probe each of these states selectively and determine the respective transient populations depending on optical laser fluence. Ab initio molecular dynamics simulations of CO adsorbed on Ru(0001) were performed at 1500 and 3000 K providing insight into the desorption process.

Ultrafast optical spectroscopy of single-walled carbon nanotubes

NASA Astrophysics Data System (ADS)

Ostojic, Gordana

Wavelength-dependent, near-infrared pump-probe study of micelle-suspended Single-Walled Carbon Nanotubes (SWCNTs) whose linear absorption spectra show chirality-assigned peaks is presented. Two distinct relaxation regimes were observed: fast (0.3--1.2 ps) and slow (5--20 ps). The slow component, which has previously been unobserved in pump-probe measurements of bundled tubes, was resonantly enhanced whenever the pump photon energy matched with an interband absorption peak, and it is attributed to interband carrier recombination. It represents the lower limit of the intrinsic radiative recombination time of photoexcited carriers in SWCNTs since the exact value of this parameter depends on the presence of possible nonradiative recombination channels. The slow decay component was highly dependent on the pH of the solution, suggesting that the surrounding H+ ions strongly affect electronic states in nanotubes through the Burnstein-Moss effect. The effect was bandgap energy dependent, affecting the smaller bandgap tubes more significantly. To elucidate carrier dynamics in more detail, nondegenerate pump-probe experiments with wide and continuum probing throughout the lowest and second lowest energy transition ranges of SWCNTs were used. Complex signals were revealed with photoinduced absorption and bleaching, both of which were strongly wavelength dependent. Due to the high optical quality of unbundled SWCNT samples, clear signs of band filling and broadening of the exciton absorption peaks were found to be the main nonlinear mechanisms. The identification of these nonlinear mechanisms presents a novel explanation of the observed nonlinear behavior of nanotubes in general and helps clarify the controversial issues presented in previously published work. This explanation is also consistent with the previously observed pump-probe signals in bundled nanotube samples. Another novel and important conclusion drawn from the nondegenerate pump-probe experiments is that the

Circularly polarized attosecond pulse generation and applications to ultrafast magnetism

NASA Astrophysics Data System (ADS)

Bandrauk, André D.; Guo, Jing; Yuan, Kai-Jun

2017-12-01

Attosecond science is a growing new field of research and potential applications which relies on the development of attosecond light sources. Achievements in the generation and application of attosecond pulses enable to investigate electron dynamics in the nonlinear nonperturbative regime of laser-matter interactions on the electron’s natural time scale, the attosecond. In this review, we describe the generation of circularly polarized attosecond pulses and their applications to induce attosecond magnetic fields, new tools for ultrafast magnetism. Simulations are performed on aligned one-electron molecular ions by using nonperturbative nonlinear solutions of the time-dependent Schrödinger equation. We discuss how bichromatic circularly polarized laser pulses with co-rotating or counter-rotating components induce electron-parent ion recollisions, thus producing circularly polarized high-order harmonic generation, the source of circularly polarized attosecond pulses. Ultrafast quantum electron currents created by the generated attosecond pulses give rise to attosecond magnetic field pulses. The results provide a guiding principle for producing circularly polarized attosecond pulses and ultrafast magnetic fields in complex molecular systems for future research in ultrafast magneto-optics.

Linear and nonlinear optical characteristics of Te nanoparticles-doped germanate glasses

NASA Astrophysics Data System (ADS)

Xu, Zhousu; Guo, Qiangbing; Liu, Chang; Ma, Zhijun; Liu, Xiaofeng; Qiu, Jianrong

2016-10-01

Te nanoparticles (NPs)-doped GeO2-MgO-B2O3-Al2O3-TeO2 glasses were prepared by the conventional melt-quenching method. Based on X-ray photoelectron spectroscopy, Raman spectroscopy and transmission electron microscope observation, the coloration of the glass at high TeO2 concentration is ascribed to the precipitation of elemental Te NPs with a size of 5-10 nm in the germanate glass. Optical absorption spectra and nonlinear optical (NLO) properties of the glass samples were analyzed by UV-3600 spectrophotometry and Z-scan technique, respectively. The nonlinear absorption coefficient ( β) and the imaginary part of the third-order NLO susceptibility (Im χ (3)) were estimated to be 1.74 cm/GW and 1.142 × 10-12 esu for laser power of 95 μW, respectively. Due to the excellent NLO properties, the Te NPs-doped germanate glasses may have potential applications for ultrafast optical switch and photonics.

Ultra-fast framing camera tube

DOEpatents

Kalibjian, Ralph

1981-01-01

An electronic framing camera tube features focal plane image dissection and synchronized restoration of the dissected electron line images to form two-dimensional framed images. Ultra-fast framing is performed by first streaking a two-dimensional electron image across a narrow slit, thereby dissecting the two-dimensional electron image into sequential electron line images. The dissected electron line images are then restored into a framed image by a restorer deflector operated synchronously with the dissector deflector. The number of framed images on the tube's viewing screen is equal to the number of dissecting slits in the tube. The distinguishing features of this ultra-fast framing camera tube are the focal plane dissecting slits, and the synchronously-operated restorer deflector which restores the dissected electron line images into a two-dimensional framed image. The framing camera tube can produce image frames having high spatial resolution of optical events in the sub-100 picosecond range.

Efficient two-stage dual-beam noncollinear optical parametric amplifier

NASA Astrophysics Data System (ADS)

Cheng, Yu-Hsiang; Gao, Frank Y.; Poulin, Peter R.; Nelson, Keith A.

2018-06-01

We have constructed a noncollinear optical parametric amplifier with two signal beams amplified in the same nonlinear crystal. This dual-beam design is more energy-efficient than operating two amplifiers in parallel. The cross-talk between two beams has been characterized and discussed. We have also added a second amplification stage to enhance the output of one of the arms, which is then frequency-doubled for ultraviolet generation. This single device provides two tunable sources for ultrafast spectroscopy in the ultraviolet and visible region.

Phase Recovery Acceleration of Quantum-Dot Semiconductor Optical Amplifiers by Optical Pumping to Quantum-Well Wetting Layer

NASA Astrophysics Data System (ADS)

Kim, Jungho

2013-11-01

We theoretically investigate the phase recovery acceleration of quantum-dot (QD) semiconductor optical amplifiers (SOAs) by means of the optical pump injection to the quantum-well (QW) wetting layer (WL). We compare the ultrafast gain and phase recovery responses of QD SOAs in either the electrical or the optical pumping scheme by numerically solving 1088 coupled rate equations. The ultrafast gain recovery responses on the order of sub-picosecond are nearly the same for the two pumping schemes. The ultrafast phase recovery is not significantly accelerated by increasing the electrical current density, but greatly improved by increasing the optical pumping power to the QW WL. Because the phase recovery time of QD SOAs with the optical pumping scheme can be reduced down to several picoseconds, the complete phase recovery can be achieved when consecutive pulse signals with a repetition rate of 100 GHz is injected.

Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling

DOE PAGES

Abraham, Baxter; Nieto-Pescador, Jesus; Gundlach, Lars

2016-08-02

Cyclic tetrapyrroles are the active core of compounds with crucial roles in living systems, such as hemoglobin and chlorophyll, and in technology as photocatalysts and light absorbers for solar energy conversion. Zinc-tetraphenylporphyrin (Zn-TPP) is a prototypical cyclic tetrapyrrole that has been intensely studied in past decades. Because of its importance for photochemical processes the optical properties are of particular interest, and, accordingly, numerous studies have focused on light absorption and excited-state dynamics of Zn-TPP. Relaxation after photoexcitation in the Soret band involves internal conversion that is preceded by an ultrafast process. This relaxation process has been observed by several groups.more » Until now, it has not been established if it involves a higher lying ”dark” state or vibrational relaxation in the excited S 2 state. Here we combine high time resolution electronic and vibrational spectroscopy to show that this process constitutes vibrational relaxation in the anharmonic 2 potential.« less

Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling

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

Abraham, Baxter; Nieto-Pescador, Jesus; Gundlach, Lars

Cyclic tetrapyrroles are the active core of compounds with crucial roles in living systems, such as hemoglobin and chlorophyll, and in technology as photocatalysts and light absorbers for solar energy conversion. Zinc-tetraphenylporphyrin (Zn-TPP) is a prototypical cyclic tetrapyrrole that has been intensely studied in past decades. Because of its importance for photochemical processes the optical properties are of particular interest, and, accordingly, numerous studies have focused on light absorption and excited-state dynamics of Zn-TPP. Relaxation after photoexcitation in the Soret band involves internal conversion that is preceded by an ultrafast process. This relaxation process has been observed by several groups.more » Until now, it has not been established if it involves a higher lying ”dark” state or vibrational relaxation in the excited S 2 state. Here we combine high time resolution electronic and vibrational spectroscopy to show that this process constitutes vibrational relaxation in the anharmonic 2 potential.« less

Nanosystems in ultrafast and superstrong fields: attosecond phenomena (Conference Presentation)

NASA Astrophysics Data System (ADS)

Stockman, Mark I.

2017-02-01

We present our latest results for a new class of phenomena in condensed matter nanooptics when a strong optical field ˜1-3 V/Å changes a solid within optical cycle [1-8]. Such a pulse drives ampere-scale currents in dielectrics and adiabatically controls their properties, including optical absorption and reflection, extreme UV absorption, and generation of high harmonics [9] in a non-perturbative manner on a 100-as temporal scale. Applied to a metal, such a pulse causes an instantaneous and, potentially, reversible change from the metallic to semimetallic properties. We will also discuss our latest theoretical results on graphene that in a strong ultrashort pulse field exhibits unique behavior [10-12]. New phenomena are predicted for buckled two-dimensional solids, silicene and germanene [13]. These are fastest phenomena in optics unfolding within half period of light. They offer potential for petahertz-bandwidth signal processing, generation of high harmonics on a nanometer spatial scale, etc. References 1. M. Durach, A. Rusina, M. F. Kling, and M. I. Stockman, Metallization of Nanofilms in Strong Adiabatic Electric Fields, Phys. Rev. Lett. 105, 086803-1-4 (2010). 2. M. Durach, A. Rusina, M. F. Kling, and M. I. Stockman, Predicted Ultrafast Dynamic Metallization of Dielectric Nanofilms by Strong Single-Cycle Optical Fields, Phys. Rev. Lett. 107, 086602-1-5 (2011). 3. A. Schiffrin, T. Paasch-Colberg, N. Karpowicz, V. Apalkov, D. Gerster, S. Muhlbrandt, M. Korbman, J. Reichert, M. Schultze, S. Holzner, J. V. Barth, R. Kienberger, R. Ernstorfer, V. S. Yakovlev, M. I. Stockman, and F. Krausz, Optical-Field-Induced Current in Dielectrics, Nature 493, 70-74 (2013). 4. M. Schultze, E. M. Bothschafter, A. Sommer, S. Holzner, W. Schweinberger, M. Fiess, M. Hofstetter, R. Kienberger, V. Apalkov, V. S. Yakovlev, M. I. Stockman, and F. Krausz, Controlling Dielectrics with the Electric Field of Light, Nature 493, 75-78 (2013). 5. V. Apalkov and M. I. Stockman, Metal Nanofilm

Two-Dimensional CH3NH3PbI3 Perovskite Nanosheets for Ultrafast Pulsed Fiber Lasers.

PubMed

Li, Pengfei; Chen, Yao; Yang, Tieshan; Wang, Ziyu; Lin, Han; Xu, Yanhua; Li, Lei; Mu, Haoran; Shivananju, Bannur Nanjunda; Zhang, Yupeng; Zhang, Qinglin; Pan, Anlian; Li, Shaojuan; Tang, Dingyuan; Jia, Baohua; Zhang, Han; Bao, Qiaoliang

2017-04-12

Even though the nonlinear optical effects of solution processed organic-inorganic perovskite films have been studied, the nonlinear optical properties in two-dimensional (2D) perovskites, especially their applications for ultrafast photonics, are largely unexplored. In comparison to bulk perovskite films, 2D perovskite nanosheets with small thicknesses of a few unit cells are more suitable for investigating the intrinsic nonlinear optical properties because bulk recombination of photocarriers and the nonlinear scattering are relatively small. In this research, we systematically investigated the nonlinear optical properties of 2D perovskite nanosheets derived from a combined solution process and vapor phase conversion method. It was found that 2D perovskite nanosheets have stronger saturable absorption properties with large modulation depth and very low saturation intensity compared with those of bulk perovskite films. Using an all dry transfer method, we constructed a new type of saturable absorber device based on single piece 2D perovskite nanosheet. Stable soliton state mode-locking was achieved, and ultrafast picosecond pulses were generated at 1064 nm. This work is likely to pave the way for ultrafast photonic and optoelectronic applications based on 2D perovskites.

Ultrafast Laser Beam Switching and Pulse Train Generation by Using Coupled Vertical-Cavity, Surface-Emitting Lasers (VCSELS)

NASA Technical Reports Server (NTRS)

Goorjian, Peter M. (Inventor); Ning, Cun-Zheng (Inventor)

2005-01-01

Ultrafast directional beam switching is achieved using coupled VCSELs. This approach is demonstrated to achieve beam switching frequencies of 40 GHz and more and switching directions of about eight degrees. This switching scheme is likely to be useful for ultrafast optical networks at frequencies much higher than achievable with other approaches.

Optical spectroscopy using gas-phase femtosecond laser filamentation.

PubMed

Odhner, Johanan; Levis, Robert

2014-01-01

Femtosecond laser filamentation occurs as a dynamic balance between the self-focusing and plasma defocusing of a laser pulse to produce ultrashort radiation as brief as a few optical cycles. This unique source has many properties that make it attractive as a nonlinear optical tool for spectroscopy, such as propagation at high intensities over extended distances, self-shortening, white-light generation, and the formation of an underdense plasma. The plasma channel that constitutes a single filament and whose position in space can be controlled by its input parameters can span meters-long distances, whereas multifilamentation of a laser beam can be sustained up to hundreds of meters in the atmosphere. In this review, we briefly summarize the current understanding and use of laser filaments for spectroscopic investigations of molecules. A theoretical framework of filamentation is presented, along with recent experimental evidence supporting the established understanding of filamentation. Investigations carried out on vibrational and rotational spectroscopy, filament-induced breakdown, fluorescence spectroscopy, and backward lasing are discussed.

Collimating slicer for optical integral field spectroscopy

NASA Astrophysics Data System (ADS)

Laurent, Florence; Hénault, François

2016-07-01

Integral Field Spectroscopy (IFS) is a technique that gives simultaneously the spectrum of each spatial sampling element of a given field. It is a powerful tool which rearranges the data cube represented by two spatial dimensions defining the field and the spectral decomposition (x, y, λ) in a detector plane. In IFS, the "spatial" unit reorganizes the field, the "spectral" unit is being composed of a classical spectrograph. For the spatial unit, three main techniques - microlens array, microlens array associated with fibres and image slicer - are used in astronomical instrumentations. The development of a Collimating Slicer is to propose a new type of optical integral field spectroscopy which should be more compact. The main idea is to combine the image slicer with the collimator of the spectrograph mixing the "spatial" and "spectral" units. The traditional combination of slicer, pupil and slit elements and spectrograph collimator is replaced by a new one composed of a slicer and spectrograph collimator only. After testing few configurations, this new system looks very promising for low resolution spectrographs. In this paper, the state of art of integral field spectroscopy using image slicers will be described. The new system based onto the development of a Collimating Slicer for optical integral field spectroscopy will be depicted. First system analysis results and future improvements will be discussed.

Compressive sensing for single-shot two-dimensional coherent spectroscopy

NASA Astrophysics Data System (ADS)

Harel, E.; Spencer, A.; Spokoyny, B.

2017-02-01

In this work, we explore the use of compressive sensing for the rapid acquisition of two-dimensional optical spectra that encodes the electronic structure and ultrafast dynamics of condensed-phase molecular species. Specifically, we have developed a means to combine multiplexed single-element detection and single-shot and phase-resolved two-dimensional coherent spectroscopy. The method described, which we call Single Point Array Reconstruction by Spatial Encoding (SPARSE) eliminates the need for costly array detectors while speeding up acquisition by several orders of magnitude compared to scanning methods. Physical implementation of SPARSE is facilitated by combining spatiotemporal encoding of the nonlinear optical response and signal modulation by a high-speed digital micromirror device. We demonstrate the approach by investigating a well-characterized cyanine molecule and a photosynthetic pigment-protein complex. Hadamard and compressive sensing algorithms are demonstrated, with the latter achieving compression factors as high as ten. Both show good agreement with directly detected spectra. We envision a myriad of applications in nonlinear spectroscopy using SPARSE with broadband femtosecond light sources in so-far unexplored regions of the electromagnetic spectrum.

Spectroscopy and optical imaging of coalescing droplets

NASA Astrophysics Data System (ADS)

Ivanov, Maksym; Viderström, Michel; Chang, Kelken; Ramírez Contreras, Claudia; Mehlig, Bernhard; Hanstorp, Dag

2016-09-01

We report on experimental investigations of the dynamics of colliding liquid droplets by combining optical trapping, spectroscopy and high-speed color imaging. Two droplets with diameters between 5 and 50 microns are suspended in quiescent air by optical traps. The traps allows us to control the initial positions, and hence the impact parameter and the relative velocity of the colliding droplets. Movies of the droplet dynamics are recorded using high-speed digital movie cameras at a frame rate of up to 63000 frames per second. A fluorescent dye is added to one of the colliding droplets. We investigate the temporal evolution of the scattered and fluorescence light from the colliding droplets with concurrent spectroscopy and color imaging. This technique can be used to detect the exchange of molecules between a pair of neutral or charged droplets.

A New Optical Design for Imaging Spectroscopy

NASA Astrophysics Data System (ADS)

Thompson, K. L.

2002-05-01

We present an optical design concept for imaging spectroscopy, with some advantages over current systems. The system projects monochromatic images onto the 2-D array detector(s). Faint object and crowded field spectroscopy can be reduced first using image processing techniques, then building the spectrum, unlike integral field units where one must first extract the spectra, build data cubes from these, then reconstruct the target's integrated spectral flux. Like integral field units, all photons are detected simultaneously, unlike tunable filters which must be scanned through the wavelength range of interest and therefore pay a sensitivity pentalty. Several sample designs are presented, including an instrument optimized for measuring intermediate redshift galaxy cluster velocity dispersions, one designed for near-infrared ground-based adaptive optics, and one intended for space-based rapid follow-up of transient point sources such as supernovae and gamma ray bursts.

A Dual-Colour Architecture for Pump-Probe Spectroscopy of Ultrafast Magnetization Dynamics in the Sub-10-femtosecond Range.

PubMed

Gonçalves, C S; Silva, A S; Navas, D; Miranda, M; Silva, F; Crespo, H; Schmool, D S

2016-03-15

Current time-resolution-limited dynamic measurements clearly show the need for improved techniques to access processes on the sub-10-femtosecond timescale. To access this regime, we have designed and constructed a state-of-the-art time-resolved magneto-optic Kerr effect apparatus, based on a new dual-color scheme, for the measurement of ultrafast demagnetization and precessional dynamics in magnetic materials. This system can operate well below the current temporal ranges reported in the literature, which typically lie in the region of around 50 fs and above. We have used a dual-colour scheme, based on ultra broadband hollow-core fibre and chirped mirror pulse compression techniques, to obtain unprecedented sub-8-fs pump and probe pulse durations at the sample plane. To demonstrate the capabilities of this system for ultrafast demagnetization and precessional dynamics studies, we have performed measurements in a ferrimagnetic GdFeCo thin film. Our study has shown that the magnetization shows a sudden drop within the first picosecond after the pump pulse, a fast recovery (remagnetization) within a few picoseconds, followed by a clear oscillation or precession during a slower magnetization recovery. Moreover, we have experimentally confirmed for the first time that a sub-10-fs pulse is able to efficiently excite a magnetic system such as GdFeCo.

Optical spectroscopy techniques can accurately distinguish benign and malignant renal tumours.

PubMed

Couapel, Jean-Philippe; Senhadji, Lotfi; Rioux-Leclercq, Nathalie; Verhoest, Grégory; Lavastre, Olivier; de Crevoisier, Renaud; Bensalah, Karim

2013-05-01

WHAT'S KNOWN ON THE SUBJECT? AND WHAT DOES THE STUDY ADD?: There is little known about optical spectroscopy techniques ability to evaluate renal tumours. This study shows for the first time the ability of Raman and optical reflectance spectroscopy to distinguish benign and malignant renal tumours in an ex vivo environment. We plan to develop this optical assistance in the operating room in the near future. To evaluate the ability of Raman spectroscopy (RS) and optical reflectance spectroscopy (ORS) to distinguish benign and malignant renal tumours at surgery. Between March and October 2011, RS and ORS spectra were prospectively acquired on surgical renal specimens removed for suspicion of renal cell carcinoma (RCC). Optical measurements were done immediately after surgery. Optical signals were normalised to ensure comparison between spectra. Initial and final portions of each spectrum were removed to avoid artefacts. A support vector machine (SVM) was built and tested using a leave-one-out cross-validation. Classification scores, including accuracy, sensitivity and specificity were calculated on the entire population and in patients with tumours of <4 cm. In all, 60 nephrectomies were performed for 53 malignant tumours (41 clear-cell, eight papillary and four chromophobe carcinomas) and seven benign tumours (four oncocytomas, two angiomyolipomas and a haemorrhagic cyst). In all, >700 optical spectra were obtained and submitted to SVM classification. The SVM could recognise benign and malignant renal tumours with an accuracy of 96% (RS) and 88% (ORS) in the whole population and with an accuracy of 93% (RS) and 95% (ORS) in the present subset of small renal tumours (<4 cm). Histological subtype could be determined in 80% and 88% of the cases with RS and ORS, respectively. The SVM was able to differentiate chromophobe carcinomas and benign lesions with an accuracy of 96% in RS and 98% in ORS. Benign and malignant renal tumours can be accurately discriminated by a

Phosphorene quantum dot saturable absorbers for ultrafast fiber lasers

PubMed Central

Du, J.; Zhang, M.; Guo, Z.; Chen, J.; Zhu, X.; Hu, G.; Peng, P.; Zheng, Z.; Zhang, H.

2017-01-01

We fabricate ultrasmall phosphorene quantum dots (PQDs) with an average size of 2.6 ± 0.9 nm using a liquid exfoliation method involving ultrasound probe sonication followed by bath sonication. By coupling the as-prepared PQDs with microfiber evanescent light field, the PQD-based saturable absorber (SA) device exhibits ultrafast nonlinear saturable absorption property, with an optical modulation depth of 8.1% at the telecommunication band. With the integration of the all-fiber PQD-based SA, a continuous-wave passively mode-locked erbium-doped (Er-doped) laser cavity delivers stable, self-starting pulses with a pulse duration of 0.88 ps and at the cavity repetition rate of 5.47 MHz. Our results contribute to the growing body of work studying the nonlinear optical properties of ultrasmall PQDs that present new opportunities of this two-dimensional (2D) nanomaterial for future ultrafast photonic technologies. PMID:28211471

Mapping carrier diffusion in single silicon core-shell nanowires with ultrafast optical microscopy.

PubMed

Seo, M A; Yoo, J; Dayeh, S A; Picraux, S T; Taylor, A J; Prasankumar, R P

2012-12-12

Recent success in the fabrication of axial and radial core-shell heterostructures, composed of one or more layers with different properties, on semiconductor nanowires (NWs) has enabled greater control of NW-based device operation for various applications. (1-3) However, further progress toward significant performance enhancements in a given application is hindered by the limited knowledge of carrier dynamics in these structures. In particular, the strong influence of interfaces between different layers in NWs on transport makes it especially important to understand carrier dynamics in these quasi-one-dimensional systems. Here, we use ultrafast optical microscopy (4) to directly examine carrier relaxation and diffusion in single silicon core-only and Si/SiO(2) core-shell NWs with high temporal and spatial resolution in a noncontact manner. This enables us to reveal strong coherent phonon oscillations and experimentally map electron and hole diffusion currents in individual semiconductor NWs for the first time.

Femtosecond coherent nuclear dynamics of excited tetraphenylethylene: Ultrafast transient absorption and ultrafast Raman loss spectroscopic studies

NASA Astrophysics Data System (ADS)

Kayal, Surajit; Roy, Khokan; Umapathy, Siva

2018-01-01

Ultrafast torsional dynamics plays an important role in the photoinduced excited state dynamics. Tetraphenylethylene (TPE), a model system for the molecular motor, executes interesting torsional dynamics upon photoexcitation. The photoreaction of TPE involves ultrafast internal conversion via a nearly planar intermediate state (relaxed state) that further leads to a twisted zwitterionic state. Here, we report the photoinduced structural dynamics of excited TPE during the course of photoisomerization in the condensed phase by ultrafast Raman loss (URLS) and femtosecond transient absorption (TA) spectroscopy. TA measurements on the S1 state reveal step-wise population relaxation from the Franck-Condon (FC) state → relaxed state → twisted state, while the URLS study provides insights on the vibrational dynamics during the course of the reaction. The TA spectral dynamics and vibrational Raman amplitudes within 1 ps reveal vibrational wave packet propagating from the FC state to the relaxed state. Fourier transformation of this oscillation leads to a ˜130 cm-1 low-frequency phenyl torsional mode. Two vibrational marker bands, Cet=Cet stretching (˜1512 cm-1) and Cph=Cph stretching (˜1584 cm-1) modes, appear immediately after photoexcitation in the URLS spectra. The initial red-shift of the Cph=Cph stretching mode with a time constant of ˜400 fs (in butyronitrile) is assigned to the rate of planarization of excited TPE. In addition, the Cet=Cet stretching mode shows initial blue-shift within 1 ps followed by frequency red-shift, suggesting that on the sub-picosecond time scale, structural relaxation is dominated by phenyl torsion rather than the central Cet=Cet twist. Furthermore, the effect of the solvent on the structural dynamics is discussed in the context of ultrafast nuclear dynamics and solute-solvent coupling.

Femtosecond coherent nuclear dynamics of excited tetraphenylethylene: Ultrafast transient absorption and ultrafast Raman loss spectroscopic studies.

PubMed

Kayal, Surajit; Roy, Khokan; Umapathy, Siva

2018-01-14

Ultrafast torsional dynamics plays an important role in the photoinduced excited state dynamics. Tetraphenylethylene (TPE), a model system for the molecular motor, executes interesting torsional dynamics upon photoexcitation. The photoreaction of TPE involves ultrafast internal conversion via a nearly planar intermediate state (relaxed state) that further leads to a twisted zwitterionic state. Here, we report the photoinduced structural dynamics of excited TPE during the course of photoisomerization in the condensed phase by ultrafast Raman loss (URLS) and femtosecond transient absorption (TA) spectroscopy. TA measurements on the S 1 state reveal step-wise population relaxation from the Franck-Condon (FC) state → relaxed state → twisted state, while the URLS study provides insights on the vibrational dynamics during the course of the reaction. The TA spectral dynamics and vibrational Raman amplitudes within 1 ps reveal vibrational wave packet propagating from the FC state to the relaxed state. Fourier transformation of this oscillation leads to a ∼130 cm -1 low-frequency phenyl torsional mode. Two vibrational marker bands, C et =C et stretching (∼1512 cm -1 ) and C ph =C ph stretching (∼1584 cm -1 ) modes, appear immediately after photoexcitation in the URLS spectra. The initial red-shift of the C ph =C ph stretching mode with a time constant of ∼400 fs (in butyronitrile) is assigned to the rate of planarization of excited TPE. In addition, the C et =C et stretching mode shows initial blue-shift within 1 ps followed by frequency red-shift, suggesting that on the sub-picosecond time scale, structural relaxation is dominated by phenyl torsion rather than the central C et =C et twist. Furthermore, the effect of the solvent on the structural dynamics is discussed in the context of ultrafast nuclear dynamics and solute-solvent coupling.

AXSIS: Exploring the frontiers in attosecond X-ray science, imaging and spectroscopy.

PubMed

Kärtner, F X; Ahr, F; Calendron, A-L; Çankaya, H; Carbajo, S; Chang, G; Cirmi, G; Dörner, K; Dorda, U; Fallahi, A; Hartin, A; Hemmer, M; Hobbs, R; Hua, Y; Huang, W R; Letrun, R; Matlis, N; Mazalova, V; Mücke, O D; Nanni, E; Putnam, W; Ravi, K; Reichert, F; Sarrou, I; Wu, X; Yahaghi, A; Ye, H; Zapata, L; Zhang, D; Zhou, C; Miller, R J D; Berggren, K K; Graafsma, H; Meents, A; Assmann, R W; Chapman, H N; Fromme, P

2016-09-01

X-ray crystallography is one of the main methods to determine atomic-resolution 3D images of the whole spectrum of molecules ranging from small inorganic clusters to large protein complexes consisting of hundred-thousands of atoms that constitute the macromolecular machinery of life. Life is not static, and unravelling the structure and dynamics of the most important reactions in chemistry and biology is essential to uncover their mechanism. Many of these reactions, including photosynthesis which drives our biosphere, are light induced and occur on ultrafast timescales. These have been studied with high time resolution primarily by optical spectroscopy, enabled by ultrafast laser technology, but they reduce the vast complexity of the process to a few reaction coordinates. In the AXSIS project at CFEL in Hamburg, funded by the European Research Council, we develop the new method of attosecond serial X-ray crystallography and spectroscopy, to give a full description of ultrafast processes atomically resolved in real space and on the electronic energy landscape, from co-measurement of X-ray and optical spectra, and X-ray diffraction. This technique will revolutionize our understanding of structure and function at the atomic and molecular level and thereby unravel fundamental processes in chemistry and biology like energy conversion processes. For that purpose, we develop a compact, fully coherent, THz-driven atto-second X-ray source based on coherent inverse Compton scattering off a free-electron crystal, to outrun radiation damage effects due to the necessary high X-ray irradiance required to acquire diffraction signals. This highly synergistic project starts from a completely clean slate rather than conforming to the specifications of a large free-electron laser (FEL) user facility, to optimize the entire instrumentation towards fundamental measurements of the mechanism of light absorption and excitation energy transfer. A multidisciplinary team formed by laser

Ultrafast magneto-optical spectroscopy of GaMnAs (Invited Paper)

NASA Astrophysics Data System (ADS)

Heroux, Jean Benoit; Kojima, Eiji; Ino, Y.; Hashimoto, Y.; Katsumoto, Shingo; Iye, Yasushiro; Kuwata-Gonokami, Makoto

2005-04-01

Spin dynamics in the III-V dilute magnetic semiconductor GaMnAs is investigated by photo-induced demagnetization. Experimental results obtained from two different time-dependent characterization techniques - "two color-probe" magneto-optical Kerr effect (TR-MOKE) and mid-infrared differential transmittance -- are compared. Upon photo-excitation with a 100 fs, 3.1 eV light pulse, a long demagnetization time in the hundreds of picoseconds timescale is found by TR-MOKE, indicating a spin-dependent band structure in this material. In mid-infrared measurements, a positive increase of the differential transmittance is observed in the same time interval when the sample is cooled below its Currie temperature. It is shown that this mid-infrared absorption feature is directly related to ferromagnetism in this material. The magnetism-related component of the broad DC mid-infrared absorption peak characteristic of this p-type material could be observed with this time-resolved measurement. Experimental results were simulated with a model describing the interaction between three thermal reservoirs (hole, spin and lattice) and taking thermal diffusion into account.

Versatile multi-wavelength ultrafast fiber laser mode-locked by carbon nanotubes

PubMed Central

Liu, Xueming; Han, Dongdong; Sun, Zhipei; Zeng, Chao; Lu, Hua; Mao, Dong; Cui, Yudong; Wang, Fengqiu

2013-01-01

Multi-wavelength lasers have widespread applications (e.g. fiber telecommunications, pump-probe measurements, terahertz generation). Here, we report a nanotube-mode-locked all-fiber ultrafast oscillator emitting three wavelengths at the central wavelengths of about 1540, 1550, and 1560 nm, which are tunable by stretching fiber Bragg gratings. The output pulse duration is around 6 ps with a spectral width of ~0.5 nm, agreeing well with the numerical simulations. The triple-laser system is controlled precisely and insensitive to environmental perturbations with <0.04% amplitude fluctuation. Our method provides a simple, stable, low-cost, multi-wavelength ultrafast-pulsed source for spectroscopy, biomedical research and telecommunications. PMID:24056500

Generalized Kramers-Kronig relations in nonlinear optical- and THz-spectroscopy

NASA Astrophysics Data System (ADS)

Peiponen, K.-E.; Saarinen, J. J.

2009-05-01

Kramers-Kronig (K-K) relations have constituted one of the principal tools in the optical spectroscopy for the assessment of the optical properties of media from measured spectra. The underlying principle for the existence of the K-K relations is causality. Thanks to the K-K relations we have achieved a better understanding of both macroscopic and microscopic properties of media. Recently, various kinds of modified K-K relations have been presented in the literature. Such relations have been applied, e.g. to the nonlinear optical properties of polymers. A typical advantage of these generalized K-K relations is that the measured data do not need to be manipulated as in the case of the traditional K-K relations. Hence, the accuracy of the inverted data on linear or nonlinear optical properties of media becomes higher. A novel way to utilize generalized K-K relations is related to the measurement and correction of terahertz spectra in the time-domain reflection spectroscopy. Terahertz spectroscopy is nowadays one of the most rapidly developing fields in modern physics with applications being related to, e.g. security at the airports or inspection of pharmaceutical tablets. While recording THz spectra it is also possible to perform a chemical mapping of species. Therefore, correctness of the spectrum is of crucial importance for the identification of different species. This is possible by the generalized K-K relations. In this review paper we consider advances of K-K relations both in nonlinear optical and THz spectroscopy.

Doppler-free spectroscopy of the atomic rubidium fine structure using ultrafast spatial coherent control method

NASA Astrophysics Data System (ADS)

Kim, Minhyuk; Kim, Kyungtae; Lee, Woojun; Kim, Hyosub; Ahn, Jaewook

2017-04-01

Spectral programming solutions for the ultrafast spatial coherent control (USCC) method to resolve the fine-structure energy levels of atomic rubidium are reported. In USCC, a pair of counter-propagating ultrashort laser pulses are programmed to make a two-photon excitation pattern specific to particular transition pathways and atom species, thus allowing the involved transitions resolvable in space simultaneously. With a proper spectral phase and amplitude modulation, USCC has been also demonstrated for the systems with many intermediate energy levels. Pushing the limit of system complexity even further, we show here an experimental demonstration of the rubidium fine-structure excitation pattern resolvable by USCC. The spectral programming solution for the given USCC is achieved by combining a double-V-shape spectral phase function and a set of phase steps, where the former distinguishes the fine structure and the latter prevents resonant transitions. The experimental results will be presented along with its application in conjunction with the Doppler-free frequency-comb spectroscopy for rubidium hyperfine structure measurements. Samsung Science and Technology Foundation [SSTFBA1301-12].

Probing Ultrafast Electron Dynamics at Surfaces Using Soft X-Ray Transient Reflectivity Spectroscopy

NASA Astrophysics Data System (ADS)

Baker, L. Robert; Husek, Jakub; Biswas, Somnath; Cirri, Anthony

The ability to probe electron dynamics with surface sensitivity on the ultrafast time scale is critical for understanding processes such as charge separation, injection, and surface trapping that mediate efficiency in catalytic and energy conversion materials. Toward this goal, we have developed a high harmonic generation (HHG) light source for femtosecond soft x-ray reflectivity. Using this light source we investigated the ultrafast carrier dynamics at the surface of single crystalline α-Fe2O3, polycrystalline α-Fe2O3, and the mixed metal oxide, CuFeO2. We have recently demonstrated that CuFeO2 in particular is a selective catalyst for photo-electrochemical CO2 reduction to acetate; however, the role of electronic structure and charge carrier dynamics in mediating catalytic selectivity has not been well understood. Soft x-ray reflectivity measurements probe the M2,3, edges of the 3d transition metals, which provide oxidation and spin state resolution with element specificity. In addition to chemical state specificity, these measurements are also surface sensitive, and by independently simulating the contributions of the real and imaginary components of the complex refractive index, we can differentiate between surface and sub-surface contributions to the excited state spectrum. Accordingly, this work demonstrates the ability to probe ultrafast carrier dynamics in catalytic materials with element and chemical state specificity and with surface sensitivity.

Real-time visualization of soliton molecules with evolving behavior in an ultrafast fiber laser

NASA Astrophysics Data System (ADS)

Liu, Meng; Li, Heng; Luo, Ai-Ping; Cui, Hu; Xu, Wen-Cheng; Luo, Zhi-Chao

2018-03-01

Ultrafast fiber lasers have been demonstrated to be great platforms for the investigation of soliton dynamics. The soliton molecules, as one of the most fascinating nonlinear phenomena, have been a hot topic in the field of nonlinear optics in recent years. Herein, we experimentally observed the real-time evolving behavior of soliton molecule in an ultrafast fiber laser by using the dispersive Fourier transformation technology. Several types of evolving soliton molecules were obtained in our experiments, such as soliton molecules with monotonically or chaotically evolving phase, flipping and hopping phase. These results would be helpful to the communities interested in soliton nonlinear dynamics as well as ultrafast laser technologies.

Ultrafast, superhigh gain visible-blind UV detector and optical logic gates based on nonpolar a-axial GaN nanowire

NASA Astrophysics Data System (ADS)

Wang, Xingfu; Zhang, Yong; Chen, Xinman; He, Miao; Liu, Chao; Yin, Yian; Zou, Xianshao; Li, Shuti

2014-09-01

Nonpolar a-axial GaN nanowire (NW) was first used to construct the MSM (metal-semiconductor-metal) symmetrical Schottky contact device for application as visible-blind ultraviolet (UV) detector. Without any surface or composition modifications, the fabricated device demonstrated a superior performance through a combination of its high sensitivity (up to 104 A W-1) and EQE value (up to 105), as well as ultrafast (<26 ms) response speed, which indicates that a balance between the photocurrent gain and the response speed has been achieved. Based on its excellent photoresponse performance, an optical logic AND gate and OR gate have been demonstrated for performing photo-electronic coupled logic devices by further integrating the fabricated GaN NW detectors, which logically convert optical signals to electrical signals in real time. These results indicate the possibility of using a nonpolar a-axial GaN NW not only as a high performance UV detector, but also as a stable optical logic device, both in light-wave communications and for future memory storage.Nonpolar a-axial GaN nanowire (NW) was first used to construct the MSM (metal-semiconductor-metal) symmetrical Schottky contact device for application as visible-blind ultraviolet (UV) detector. Without any surface or composition modifications, the fabricated device demonstrated a superior performance through a combination of its high sensitivity (up to 104 A W-1) and EQE value (up to 105), as well as ultrafast (<26 ms) response speed, which indicates that a balance between the photocurrent gain and the response speed has been achieved. Based on its excellent photoresponse performance, an optical logic AND gate and OR gate have been demonstrated for performing photo-electronic coupled logic devices by further integrating the fabricated GaN NW detectors, which logically convert optical signals to electrical signals in real time. These results indicate the possibility of using a nonpolar a-axial GaN NW not only as a high

Ultrafast, large-field multiphoton microscopy based on an acousto-optic deflector and a spatial light modulator.

PubMed

Shao, Yonghong; Qin, Wan; Liu, Honghai; Qu, Junle; Peng, Xiang; Niu, Hanben; Gao, Bruce Z

2012-07-01

We present an ultrafast, large-field multiphoton excitation fluorescence microscope with high lateral and axial resolutions based on a two-dimensional (2-D) acousto-optical deflector (AOD) scanner and spatial light modulator (SLM). When a phase-only SLM is used to shape the near-infrared light from a mode-locked titanium:sapphire laser into a multifocus array including the 0-order beam, a 136 μm × 136 μm field of view is achieved with a 60× objective using a 2-D AOD scanner without any mechanical scan element. The two-photon fluorescence image of a neuronal network that was obtained using this system demonstrates that our microscopy permits observation of dynamic biological events in a large field with high-temporal and -spatial resolution.

Steering optical comb frequencies by rotating the polarization state

NASA Astrophysics Data System (ADS)

Zhang, Yanyan; Zhang, Xiaofei; Yan, Lulu; Zhang, Pan; Rao, Bingjie; Han, Wei; Guo, Wenge; Zhang, Shougang; Jiang, Haifeng

2017-12-01

Optical frequency combs, with precise control of repetition rate and carrier-envelope-offset frequency, have revolutionized many fields, such as fine optical spectroscopy, optical frequency standards, ultra-fast science research, ultra-stable microwave generation and precise ranging measurement. However, existing high bandwidth frequency control methods have small dynamic range, requiring complex hybrid control techniques. To overcome this limitation, we develop a new approach, where a home-made intra-cavity electro-optic modulator tunes polarization state of laser signal rather than only optical length of the cavity, to steer frequencies of a nonlinear-polarization-rotation mode-locked laser. By taking advantage of birefringence of the whole cavity, this approach results in not only broadband but also relative large-dynamic frequency control. Experimental results show that frequency control dynamic range increase at least one order in comparison with the traditional intra-cavity electro-optic modulator technique. In additional, this technique exhibits less side-effect than traditional frequency control methods.

In-line interferometer for broadband near-field scanning optical spectroscopy.

PubMed

Brauer, Jens; Zhan, Jinxin; Chimeh, Abbas; Korte, Anke; Lienau, Christoph; Gross, Petra

2017-06-26

We present and investigate a novel approach towards broad-bandwidth near-field scanning optical spectroscopy based on an in-line interferometer for homodyne mixing of the near field and a reference field. In scattering-type scanning near-field optical spectroscopy, the near-field signal is usually obscured by a large amount of unwanted background scattering from the probe shaft and the sample. Here we increase the light reflected from the sample by a semi-transparent gold layer and use it as a broad-bandwidth, phase-stable reference field to amplify the near-field signal in the visible and near-infrared spectral range. We experimentally demonstrate that this efficiently suppresses the unwanted background signal in monochromatic near-field measurements. For rapid acquisition of complete broad-bandwidth spectra we employ a monochromator and a fast line camera. Using this fast acquisition of spectra and the in-line interferometer we demonstrate the measurement of pure near-field spectra. The experimental observations are quantitatively explained by analytical expressions for the measured optical signals, based on Fourier decomposition of background and near field. The theoretical model and in-line interferometer together form an important step towards broad-bandwidth near-field scanning optical spectroscopy.

Nondestructive surface analysis for material research using fiber optic vibrational spectroscopy

NASA Astrophysics Data System (ADS)

Afanasyeva, Natalia I.

2001-11-01

The advanced methods of fiber optical vibrational spectroscopy (FOVS) has been developed in conjunction with interferometer and low-loss, flexible, and nontoxic optical fibers, sensors, and probes. The combination of optical fibers and sensors with Fourier Transform (FT) spectrometer has been used in the range from 2.5 to 12micrometers . This technique serves as an ideal diagnostic tool for surface analysis of numerous and various diverse materials such as complex structured materials, fluids, coatings, implants, living cells, plants, and tissue. Such surfaces as well as living tissue or plants are very difficult to investigate in vivo by traditional FT infrared or Raman spectroscopy methods. The FOVS technique is nondestructive, noninvasive, fast (15 sec) and capable of operating in remote sampling regime (up to a fiber length of 3m). Fourier transform infrared (FTIR) and Raman fiber optic spectroscopy operating with optical fibers has been suggested as a new powerful tool. These techniques are highly sensitive techniques for structural studies in material research and various applications during process analysis to determine molecular composition, chemical bonds, and molecular conformations. These techniques could be developed as a new tool for quality control of numerous materials as well as noninvasive biopsy.

Revealing the ultrafast charge carrier dynamics in organo metal halide perovskite solar cell materials using time resolved THz spectroscopy

NASA Astrophysics Data System (ADS)

Ponseca, C. S., Jr.; Sundström, V.

2016-03-01

Ultrafast charge carrier dynamics in organo metal halide perovskite has been probed using time resolved terahertz (THz) spectroscopy (TRTS). Current literature on its early time characteristics is unanimous: sub-ps charge carrier generation, highly mobile charges and very slow recombination rationalizing the exceptionally high power conversion efficiency for a solution processed solar cell material. Electron injection from MAPbI3 to nanoparticles (NP) of TiO2 is found to be sub-ps while Al2O3 NPs do not alter charge dynamics. Charge transfer to organic electrodes, Spiro-OMeTAD and PCBM, is sub-ps and few hundreds of ps respectively, which is influenced by the alignment of energy bands. It is surmised that minimizing defects/trap states is key in optimizing charge carrier extraction from these materials.

Dual-modal cancer detection based on optical pH sensing and Raman spectroscopy.

PubMed

Kim, Soogeun; Lee, Seung Ho; Min, Sun Young; Byun, Kyung Min; Lee, Soo Yeol

2017-10-01

A dual-modal approach using Raman spectroscopy and optical pH sensing was investigated to discriminate between normal and cancerous tissues. Raman spectroscopy has demonstrated the potential for in vivo cancer detection. However, Raman spectroscopy has suffered from strong fluorescence background of biological samples and subtle spectral differences between normal and disease tissues. To overcome those issues, pH sensing is adopted to Raman spectroscopy as a dual-modal approach. Based on the fact that the pH level in cancerous tissues is lower than that in normal tissues due to insufficient vasculature formation, the dual-modal approach combining the chemical information of Raman spectrum and the metabolic information of pH level can improve the specificity of cancer diagnosis. From human breast tissue samples, Raman spectra and pH levels are measured using fiber-optic-based Raman and pH probes, respectively. The pH sensing is based on the dependence of pH level on optical transmission spectrum. Multivariate statistical analysis is performed to evaluate the classification capability of the dual-modal method. The analytical results show that the dual-modal method based on Raman spectroscopy and optical pH sensing can improve the performance of cancer classification. (2017) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE).

Coherent multi-heterodyne spectroscopy using acousto-optic frequency combs.

PubMed

Durán, Vicente; Schnébelin, Cȏme; Guillet de Chatellus, Hugues

2018-05-28

We propose and characterize experimentally a new source of optical frequency combs for performing multi-heterodyne spectrometry. This comb modality is based on a frequency-shifting loop seeded with a continuous-wave (CW) monochromatic laser. The comb lines are generated by successive passes of the CW laser through an acousto-optic frequency shifter. We report the generation of frequency combs with more than 1500 mutually coherent lines, without resorting to non-linear broadening phenomena or external electronic modulation. The comb line spacing is easily reconfigurable from tens of MHz down to the kHz region. We first use a single acousto-optic frequency comb to conduct self-heterodyne interferometry with a high frequency resolution (500 kHz). By increasing the line spacing to 80 MHz, we demonstrate molecular spectroscopy on the sub-millisecond time scale. In order to reduce the detection bandwidth, we subsequently implement an acousto-optic dual-comb spectrometer with the aid of two mutually coherent frequency shifting loops. In each architecture, the potentiality of acousto-optic frequency combs for spectroscopy is validated by spectral measurements of hydrogen cyanide in the near-infrared region.

Coherent multi-heterodyne spectroscopy using acousto-optic frequency combs

NASA Astrophysics Data System (ADS)

Durán, Vicente; Schnébelin, Cȏme; Guillet de Chatellus, Hugues

2018-05-01

We propose and characterize experimentally a new source of optical frequency combs for performing multi-heterodyne spectrometry. This comb modality is based on a frequency shifting loop seeded with a CW monochromatic laser. The comb lines are generated by successive passes of the CW laser through an acousto-optic frequency shifter. We report the generation of frequency combs with more than 1500 mutually coherent lines, without resorting to non-linear broadening phenomena or external electronic modulation. The comb line spacing is easily reconfigurable from tens of MHz down to the kHz region. We first use a single acousto-optic frequency comb to conduct self-heterodyne interferometry with a high frequency resolution (500 kHz). By increasing the line spacing to 80 MHz, we demonstrate molecular spectroscopy on the sub-millisecond time scale. In order to reduce the detection bandwidth, we subsequently implement an acousto-optic dual-comb spectrometer with the aid of two mutually coherent frequency shifting loops. In each architecture, the potentiality of acousto-optic frequency combs for spectroscopy is validated by spectral measurements of hydrogen cyanide in the near-infrared region.

Advanced Ultrafast Spectroscopy for Chemical Detection of Nuclear Fuel Cycle Materials

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

Villa-Aleman, E.; Houk, A.; Spencer, W.

The development of new signatures and observables from processes related to proliferation activities are often related to the development of technologies. In our physical world, the intensity of observables is linearly related to the input drivers (light, current, voltage, etc.). Ultrafast lasers with high peak energies, opens the door to a new regime where the intensity of the observables is not necessarily linear with the laser energy. Potential nonlinear spectroscopic applications include chemical detection via remote sensing through filament generation, material characterization and processing, chemical reaction specificity, surface phenomena modifications, X-ray production, nuclear fusion, etc. The National Security Directorate lasermore » laboratory is currently working to develop new tools for nonproliferation research with femtosecond and picosecond lasers. Prior to this project, we could only achieve laser energies in the 5 nano-Joule range, preventing the study of nonlinear phenomena. To advance our nonproliferation research into the nonlinear regime we require laser pulses in the milli-Joule (mJ) energy range. We have procured and installed a 35 fs-7 mJ laser, operating at one-kilohertz repetition rate, to investigate elemental and molecular detection of materials in the laboratory with potential applications in remote sensing. Advanced, nonlinear Raman techniques will be used to study materials of interest that are in a matrix of many materials and currently with these nonlinear techniques we can achieve greater than three orders of magnitude signal enhancement. This work studying nuclear fuel cycle materials with nonlinear spectroscopies will advance SRNL research capabilities and grow a core capability within the DOE complex.« less

High-speed laser-launched flyer impacts studied with ultrafast photography and velocimetry

DOE PAGES

Banishev, Alexandr A.; Shaw, William L.; Bassett, Will P.; ...

2016-02-16

Pulsed lasers can launch thin metal foils at km s -1, but for precision measurements in shock compression science and shock wave spectroscopy, where one-dimensional shock compression is vital, flyer plate impacts with targets must have a high degree of flatness and minimal tilt, and the flyer speeds and impact times at the target must be highly reproducible. We have developed an apparatus that combines ultrafast stroboscopic optical microscopy with photon Doppler velocimetry to study impacts of laser-launched Al and Cu flyer plates with flat, transparent glass targets. The flyer plates were 0.5 mm in diameter, and ranged from 12-100more » μm thick, with flyer speeds up to 6.25 km s -1. The velocity variations over 30-60 launches from the same flyer plate optic can be as low as 0.6%, and the impact time variations can be as low as 0.8 ns. Stroboscopic image streams (reconstructed movies) show uniform, flat impacts with a glass target. As a result, these stroboscopic images can be used to estimate the tilt in the flyer-target impact to be <1mrad.« less

Ultrafast dynamics of quasiparticles and coherent acoustic phonons in slightly underdoped (BaK)Fe2As2

PubMed Central

Lin, Kung-Hsuan; Wang, Kuan-Jen; Chang, Chung-Chieh; Wen, Yu-Chieh; Lv, Bing; Chu, Ching-Wu; Wu, Maw-Kuen

2016-01-01

We have utilized ultrafast optical spectroscopy to study carrier dynamics in slightly underdoped (BaK)Fe2As2 crystals without magnetic transition. The photoelastic signals due to coherent acoustic phonons have been quantitatively investigated. According to our temperature-dependent results, we found that the relaxation component of superconducting quasiparticles persisted from the superconducting state up to at least 70 K in the normal state. Our findings suggest that the pseudogaplike feature in the normal state is possibly the precursor of superconductivity. We also highlight that the pseudogap feature of K-doped BaFe2As2 is different from that of other iron-based superconductors, including Co-doped or P-doped BaFe2As2. PMID:27180873

Evanescent-wave photoacoustic spectroscopy with optical micro/nano fibers.

PubMed

Cao, Yingchun; Jin, Wei; Ho, Lut Hoi; Liu, Zhibo

2012-01-15

We demonstrate gas detection based on evanescent-wave photoacoustic (PA) spectroscopy with tapered optical fibers. Evanescent-field instead of open-path absorption is exploited for PA generation, and a quartz tuning fork is used for PA detection. A tapered optical fiber with a diameter down to the wavelength scale demonstrates detection sensitivity similar to an open-path system but with the advantages of easier optical alignment, smaller insertion loss, and multiplexing capability.

Electron heating and thermal relaxation of gold nanorods revealed by two-dimensional electronic spectroscopy.

PubMed

Lietard, Aude; Hsieh, Cho-Shuen; Rhee, Hanju; Cho, Minhaeng

2018-03-01

To elucidate the complex interplay between the size and shape of gold nanorods and their electronic, photothermal, and optical properties for molecular imaging, photothermal therapy, and optoelectronic devices, it is a prerequisite to characterize ultrafast electron dynamics in gold nanorods. Time-resolved transient absorption (TA) studies of plasmonic electrons in various nanostructures have revealed the time scales for electron heating, lattice vibrational excitation, and phonon relaxation processes in condensed phases. However, because linear spectroscopic and time-resolved TA signals are vulnerable to inhomogeneous line-broadening, pure dephasing and direct electron heating effects are difficult to observe. Here we show that femtosecond two-dimensional electronic spectroscopy, with its unprecedented time resolution and phase sensitivity, can be used to collect direct experimental evidence for ultrafast electron heating, anomalously strong coherent and transient electronic plasmonic responses, and homogenous dephasing processes resulting from electron-vibration couplings even for polydisperse gold nanorods.

Tracking of the nuclear wavepacket motion in cyanine photoisomerization by ultrafast pump-dump-probe spectroscopy.

PubMed

Wei, Zhengrong; Nakamura, Takumi; Takeuchi, Satoshi; Tahara, Tahei

2011-06-01

Understanding ultrafast reactions, which proceed on a time scale of nuclear motions, requires a quantitative characterization of the structural dynamics. To track such structural changes with time, we studied a nuclear wavepacket motion in photoisomerization of a prototype cyanine dye, 1,1'-diethyl-4,4'-cyanine, by ultrafast pump-dump-probe measurements in solution. The temporal evolution of wavepacket motion was examined by monitoring the efficiency of stimulated emission dumping, which was obtained from the recovery of a ground-state bleaching signal. The dump efficiency versus pump-dump delay exhibited a finite rise time, and it became longer (97 fs → 330 fs → 390 fs) as the dump pulse was tuned to longer wavelengths (690 nm → 950 nm → 1200 nm). This result demonstrates a continuous migration of the leading edge of the wavepacket on the excited-state potential from the Franck-Condon region toward the potential minimum. A slowly decaying feature of the dump efficiency indicated a considerable broadening of the wavepacket over a wide range of the potential, which results in the spread of a population distribution on the flat S(1) potential energy surface. The rapid migration as well as broadening of the wavepacket manifests a continuous nature of the structural dynamics and provides an intuitive visualization of this ultrafast reaction. We also discussed experimental strategies to evaluate reliable dump efficiencies separately from other ultrafast processes and showed a high capability and possibility of the pump-dump-probe method for spectroscopic investigation of unexplored potential regions such as conical intersections. © 2011 American Chemical Society

Ultrafast dynamics in atomic clusters: Analysis and control

PubMed Central

Bonačić-Koutecký, Vlasta; Mitrić, Roland; Werner, Ute; Wöste, Ludger; Berry, R. Stephen

2006-01-01

We present a study of dynamics and ultrafast observables in the frame of pump–probe negative-to-neutral-to-positive ion (NeNePo) spectroscopy illustrated by the examples of bimetallic trimers Ag2Au−/Ag2Au/Ag2Au+ and silver oxides Ag3O2−/Ag3O2/Ag3O2+ in the context of cluster reactivity. First principle multistate adiabatic dynamics allows us to determine time scales of different ultrafast processes and conditions under which these processes can be experimentally observed. Furthermore, we present a strategy for optimal pump–dump control in complex systems based on the ab initio Wigner distribution approach and apply it to tailor laser fields for selective control of the isomerization process in Na3F2. The shapes of pulses can be assigned to underlying processes, and therefore control can be used as a tool for analysis. PMID:16740664

Ultrafast dynamics in atomic clusters: analysis and control.

PubMed

Bonacić-Koutecký, Vlasta; Mitrić, Roland; Werner, Ute; Wöste, Ludger; Berry, R Stephen

2006-07-11

We present a study of dynamics and ultrafast observables in the frame of pump-probe negative-to-neutral-to-positive ion (NeNePo) spectroscopy illustrated by the examples of bimetallic trimers Ag2Au-/Ag2Au/Ag2Au+ and silver oxides Ag3O2-/Ag3O2/Ag3O2+ in the context of cluster reactivity. First principle multistate adiabatic dynamics allows us to determine time scales of different ultrafast processes and conditions under which these processes can be experimentally observed. Furthermore, we present a strategy for optimal pump-dump control in complex systems based on the ab initio Wigner distribution approach and apply it to tailor laser fields for selective control of the isomerization process in Na3F2. The shapes of pulses can be assigned to underlying processes, and therefore control can be used as a tool for analysis.

Ultrafast collinear scattering and carrier multiplication in graphene.

PubMed

Brida, D; Tomadin, A; Manzoni, C; Kim, Y J; Lombardo, A; Milana, S; Nair, R R; Novoselov, K S; Ferrari, A C; Cerullo, G; Polini, M

2013-01-01

Graphene is emerging as a viable alternative to conventional optoelectronic, plasmonic and nanophotonic materials. The interaction of light with charge carriers creates an out-of-equilibrium distribution, which relaxes on an ultrafast timescale to a hot Fermi-Dirac distribution, that subsequently cools emitting phonons. Although the slower relaxation mechanisms have been extensively investigated, the initial stages still pose a challenge. Experimentally, they defy the resolution of most pump-probe setups, due to the extremely fast sub-100 fs carrier dynamics. Theoretically, massless Dirac fermions represent a novel many-body problem, fundamentally different from Schrödinger fermions. Here we combine pump-probe spectroscopy with a microscopic theory to investigate electron-electron interactions during the early stages of relaxation. We identify the mechanisms controlling the ultrafast dynamics, in particular the role of collinear scattering. This gives rise to Auger processes, including charge multiplication, which is key in photovoltage generation and photodetectors.

Ultrafast Photoinduced Electron Transfer in a π-Conjugated Oligomer/Porphyrin Complex.

PubMed

Aly, Shawkat M; Goswami, Subhadip; Alsulami, Qana A; Schanze, Kirk S; Mohammed, Omar F

2014-10-02

Controlling charge transfer (CT), charge separation (CS), and charge recombination (CR) at the donor-acceptor interface is extremely important to optimize the conversion efficiency in solar cell devices. In general, ultrafast CT and slow CR are desirable for optimal device performance. In this Letter, the ultrafast excited-state CT between platinum oligomer (DPP-Pt(acac)) as a new electron donor and porphyrin as an electron acceptor is monitored for the first time using femtosecond (fs) transient absorption (TA) spectroscopy with broad-band capability and 120 fs temporal resolution. Turning the CT on/off has been shown to be possible either by switching from an organometallic oligomer to a metal-free oligomer or by controlling the charge density on the nitrogen atom of the porphyrin meso unit. Our time-resolved data show that the CT and CS between DPP-Pt(acac) and cationic porphyrin are ultrafast (approximately 1.5 ps), and the CR is slow (ns time scale), as inferred from the formation and the decay of the cationic and anionic species. We also found that the metallic center in the DPP-Pt(acac) oligomer and the positive charge on the porphyrin are the keys to switching on/off the ultrafast CT process.

Raman spectroscopy: Watching a molecule breathe

NASA Astrophysics Data System (ADS)

Piatkowski, Lukasz; Hugall, James T.; van Hulst, Niek F.

2014-08-01

Marrying the single-molecule detection ability of surface-enhanced Raman scattering with the extreme time resolution of ultrafast coherent spectroscopy enables the vibrations of a single molecule to be observed.

Rippling ultrafast dynamics of suspended 2D monolayers, graphene.

PubMed

Hu, Jianbo; Vanacore, Giovanni M; Cepellotti, Andrea; Marzari, Nicola; Zewail, Ahmed H

2016-10-25

Here, using ultrafast electron crystallography (UEC), we report the observation of rippling dynamics in suspended monolayer graphene, the prototypical and most-studied 2D material. The high scattering cross-section for electron/matter interaction, the atomic-scale spatial resolution, and the ultrafast temporal resolution of UEC represent the key elements that make this technique a unique tool for the dynamic investigation of 2D materials, and nanostructures in general. We find that, at early time after the ultrafast optical excitation, graphene undergoes a lattice expansion on a time scale of 5 ps, which is due to the excitation of short-wavelength in-plane acoustic phonon modes that stretch the graphene plane. On a longer time scale, a slower thermal contraction with a time constant of 50 ps is observed and associated with the excitation of out-of-plane phonon modes, which drive the lattice toward thermal equilibrium with the well-known negative thermal expansion coefficient of graphene. From our results and first-principles lattice dynamics and out-of-equilibrium relaxation calculations, we quantitatively elucidate the deformation dynamics of the graphene unit cell.

Noncollinear wave mixing of attosecond XUV and few-cycle optical laser pulses in gas-phase atoms: Toward multidimensional spectroscopy involving XUV excitations

NASA Astrophysics Data System (ADS)

Cao, Wei; Warrick, Erika R.; Fidler, Ashley; Neumark, Daniel M.; Leone, Stephen R.

2016-11-01

Ultrafast nonlinear spectroscopy, which records transient wave-mixing signals in a medium, is a powerful tool to access microscopic information using light sources in the radio-frequency and optical regimes. The extension of this technique towards the extreme ultraviolet (XUV) or even x-ray regimes holds the promise to uncover rich structural or dynamical information with even higher spatial or temporal resolution. Here, we demonstrate noncollinear wave mixing between weak XUV attosecond pulses and a strong near-infrared (NIR) few-cycle laser pulse in gas phase atoms (one photon of XUV and two photons of NIR). In the noncollinear geometry the attosecond and either one or two NIR pulses interact with argon atoms. Nonlinear XUV signals are generated in a spatially resolved fashion as required by phase matching. Different transition pathways can be identified from these background-free nonlinear signals according to the specific phase-matching conditions. Time-resolved measurements of the spatially gated XUV signals reveal electronic coherences of Rydberg wave packets prepared by a single XUV photon or XUV-NIR two-photon excitation, depending on the applied pulse sequences. These measurements open possible applications of tabletop multidimensional spectroscopy to the study of dynamics associated with valence or core excitation with XUV photons.

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

Terahertz emission from ultrafast spin-charge current at a Rashba interface

NASA Astrophysics Data System (ADS)

Zhang, Qi; Jungfleisch, Matthias Benjamin; Zhang, Wei; Pearson, John E.; Wen, Haidan; Hoffmann, Axel

Ultrafast broadband terahertz (THz) radiation is highly desired in various fields from fundamental research in condensed matter physics to bio-chemical detection. Conventional ultrafast THz sources rely on either nonlinear optical effects or ultrafast charge currents in semiconductors. Recently, however, it was realized that ultrabroad-band THz radiation can be produced highly effectively by novel spintronics-based emitters that also make use of the electron's spin degree of freedom. Those THz-emitters convert a spin current flow into a terahertz electromagnetic pulse via the inverse spin-Hall effect. In contrast to this bulk conversion process, we demonstrate here that a femtosecond spin current pulse launched from a CoFeB layer can also generate terahertz transients efficiently at a two-dimensional Rashba interface between two non-magnetic materials, i.e., Ag/Bi. Those interfaces have been proven to be efficient means for spin- and charge current interconversion.

Quantum modeling of ultrafast photoinduced charge separation

NASA Astrophysics Data System (ADS)

Rozzi, Carlo Andrea; Troiani, Filippo; Tavernelli, Ivano

2018-01-01

Phenomena involving electron transfer are ubiquitous in nature, photosynthesis and enzymes or protein activity being prominent examples. Their deep understanding thus represents a mandatory scientific goal. Moreover, controlling the separation of photogenerated charges is a crucial prerequisite in many applicative contexts, including quantum electronics, photo-electrochemical water splitting, photocatalytic dye degradation, and energy conversion. In particular, photoinduced charge separation is the pivotal step driving the storage of sun light into electrical or chemical energy. If properly mastered, these processes may also allow us to achieve a better command of information storage at the nanoscale, as required for the development of molecular electronics, optical switching, or quantum technologies, amongst others. In this Topical Review we survey recent progress in the understanding of ultrafast charge separation from photoexcited states. We report the state-of-the-art of the observation and theoretical description of charge separation phenomena in the ultrafast regime mainly focusing on molecular- and nano-sized solar energy conversion systems. In particular, we examine different proposed mechanisms driving ultrafast charge dynamics, with particular regard to the role of quantum coherence and electron-nuclear coupling, and link experimental observations to theoretical approaches based either on model Hamiltonians or on first principles simulations.

Visualization of carrier dynamics in p(n)-type GaAs by scanning ultrafast electron microscopy

PubMed Central

Cho, Jongweon; Hwang, Taek Yong; Zewail, Ahmed H.

2014-01-01

Four-dimensional scanning ultrafast electron microscopy is used to investigate doping- and carrier-concentration-dependent ultrafast carrier dynamics of the in situ cleaved single-crystalline GaAs(110) substrates. We observed marked changes in the measured time-resolved secondary electrons depending on the induced alterations in the electronic structure. The enhancement of secondary electrons at positive times, when the electron pulse follows the optical pulse, is primarily due to an energy gain involving the photoexcited charge carriers that are transiently populated in the conduction band and further promoted by the electron pulse, consistent with a band structure that is dependent on chemical doping and carrier concentration. When electrons undergo sufficient energy loss on their journey to the surface, dark contrast becomes dominant in the image. At negative times, however, when the electron pulse precedes the optical pulse (electron impact), the dynamical behavior of carriers manifests itself in a dark contrast which indicates the suppression of secondary electrons upon the arrival of the optical pulse. In this case, the loss of energy of material’s electrons is by collisions with the excited carriers. These results for carrier dynamics in GaAs(110) suggest strong carrier–carrier scatterings which are mirrored in the energy of material’s secondary electrons during their migration to the surface. The approach presented here provides a fundamental understanding of materials probed by four-dimensional scanning ultrafast electron microscopy, and offers possibilities for use of this imaging technique in the study of ultrafast charge carrier dynamics in heterogeneously patterned micro- and nanostructured material surfaces and interfaces. PMID:24469803

Visualization of carrier dynamics in p(n)-type GaAs by scanning ultrafast electron microscopy.

PubMed

Cho, Jongweon; Hwang, Taek Yong; Zewail, Ahmed H

2014-02-11

Four-dimensional scanning ultrafast electron microscopy is used to investigate doping- and carrier-concentration-dependent ultrafast carrier dynamics of the in situ cleaved single-crystalline GaAs(110) substrates. We observed marked changes in the measured time-resolved secondary electrons depending on the induced alterations in the electronic structure. The enhancement of secondary electrons at positive times, when the electron pulse follows the optical pulse, is primarily due to an energy gain involving the photoexcited charge carriers that are transiently populated in the conduction band and further promoted by the electron pulse, consistent with a band structure that is dependent on chemical doping and carrier concentration. When electrons undergo sufficient energy loss on their journey to the surface, dark contrast becomes dominant in the image. At negative times, however, when the electron pulse precedes the optical pulse (electron impact), the dynamical behavior of carriers manifests itself in a dark contrast which indicates the suppression of secondary electrons upon the arrival of the optical pulse. In this case, the loss of energy of material's electrons is by collisions with the excited carriers. These results for carrier dynamics in GaAs(110) suggest strong carrier-carrier scatterings which are mirrored in the energy of material's secondary electrons during their migration to the surface. The approach presented here provides a fundamental understanding of materials probed by four-dimensional scanning ultrafast electron microscopy, and offers possibilities for use of this imaging technique in the study of ultrafast charge carrier dynamics in heterogeneously patterned micro- and nanostructured material surfaces and interfaces.

An ultra-fast optical shutter exploiting total light absorption in a phase change material

NASA Astrophysics Data System (ADS)

Jafari, Mohsen; Guo, L. Jay; Rais-Zadeh, Mina

2017-02-01

In this paper, we present an ultra-fast and high-contrast optical shutter with applications in atomic clock assemblies, integrated photonic systems, communication hardware, etc. The shutter design exploits the total light absorption phenomenon in a thin phase change (PC) material placed over a metal layer. The shutter switches between ON and OFF states by changing PC material phase and thus its refractive index. The PC material used in this work is Germanium Telluride (GeTe), a group IV-VI chalcogenide compound, which exhibits good optical contrast when switching from amorphous to crystalline state and vice versa. The stable phase changing behavior and reliability of GeTe and GeSbTe (GST) have been verified in optical memories and RF switches. Here, GeTe is used as it has a lower extinction coefficient in near-IR regions compared to GST. GeTe can be thermally transitioned between two phases by applying electrical pulses to an integrated heater. The memory behavior of GeTe results in zero static power consumption which is useful in applications requiring long time periods between switching activities. We previously demonstrated a meta-surface employing GeTe in sub-wavelength slits with >14 dB isolation at 1.5 μm by exciting the surface plasmon polariton and localized slit resonances. In this work, strong interference effects in a thin layer of GeTe over a gold mirror result in near total light absorption of up to 40 dB (21 dB measured) in the amorphous phase of the shutter at 780 nm with much less fabrication complexity. The optical loss at the shutter ON state is less than 1.5 dB. A nickel chrome (NiCr) heater provides the Joule heating energy required to achieve the crystallographic phase change. The measured switching speed is 2 μs.

Optical frequency comb Faraday rotation spectroscopy

NASA Astrophysics Data System (ADS)

Johansson, Alexandra C.; Westberg, Jonas; Wysocki, Gerard; Foltynowicz, Aleksandra

2018-05-01

We demonstrate optical frequency comb Faraday rotation spectroscopy (OFC-FRS) for broadband interference-free detection of paramagnetic species. The system is based on a femtosecond doubly resonant optical parametric oscillator and a fast-scanning Fourier transform spectrometer (FTS). The sample is placed in a DC magnetic field parallel to the light propagation. Efficient background suppression is implemented via switching the direction of the field on consecutive FTS scans and subtracting the consecutive spectra, which enables long-term averaging. In this first demonstration, we measure the entire Q- and R-branches of the fundamental band of nitric oxide in the 5.2-5.4 µm range and achieve good agreement with a theoretical model.

Nonlinear performance of asymmetric coupler based on dual-core photonic crystal fiber: Towards sub-nanojoule solitonic ultrafast all-optical switching

NASA Astrophysics Data System (ADS)

Curilla, L.; Astrauskas, I.; Pugzlys, A.; Stajanca, P.; Pysz, D.; Uherek, F.; Baltuska, A.; Bugar, I.

2018-05-01

We demonstrate ultrafast soliton-based nonlinear balancing of dual-core asymmetry in highly nonlinear photonic crystal fiber at sub-nanojoule pulse energy level. The effect of fiber asymmetry was studied experimentally by selective excitation and monitoring of individual fiber cores at different wavelengths between 1500 nm and 1800 nm. Higher energy transfer rate to non-excited core was observed in the case of fast core excitation due to nonlinear asymmetry balancing of temporal solitons, which was confirmed by the dedicated numerical simulations based on the coupled generalized nonlinear Schrödinger equations. Moreover, the simulation results correspond qualitatively with the experimentally acquired dependences of the output dual-core extinction ratio on excitation energy and wavelength. In the case of 1800 nm fast core excitation, narrow band spectral intensity switching between the output channels was registered with contrast of 23 dB. The switching was achieved by the change of the excitation pulse energy in sub-nanojoule region. The performed detailed analysis of the nonlinear balancing of dual-core asymmetry in solitonic propagation regime opens new perspectives for the development of ultrafast nonlinear all-optical switching devices.

Ultrafast photo-initiated molecular quantum dynamics in the DNA dinucleotide d(ApG) revealed by broadband transient absorption spectroscopy.

PubMed

Stuhldreier, Mayra C; Temps, Friedrich

2013-01-01

The ultrafast photo-initiated quantum dynamics of the adenine-guanine dinucleotide d(ApG) in aqueous solution (pH 7) has been studied by femtosecond time-resolved spectroscopy after excitation at lambda = 260 nm. The results reveal a hierarchy of processes on time scales from tau < 100 fs to tau > 100 ps. Characteristic spectro-temporal signatures are observed indicating the transformation of the molecules in the electronic relaxation from the photo-excited state to a long-lived exciplex. In particular, broadband UV/VIS excited-state absorption (ESA) measurements detected a distinctive absorption by the excited dinucleotide around lambda = 335 nm, approximately 0.5 eV to the blue compared to the maximum of the broad and unstructured ESA spectrum after excitation of an equimolar mixture of the mononucleotides dAMP and dGMP. A similar feature has been identified as signature of the excimer in the dynamics of the adenine dinucleotide d(ApA). The lifetime of the d(ApG) exciplex was found to be tau = 124 +/- 4 ps both from the ESA decay time and from the ground-state recovery time, far longer than the sub-picosecond lifetimes of excited dAMP or dGMP. Fluorescence-time profiles measured by the up-conversion technique indicate that the exciplex state is reached around approximately 6 ps after excitation. Very weak residual fluorescence at longer times red-shifted to the emission from the photo-excited state shows that the exciplex is almost optically dark, but still has enough oscillator strength to give rise to the dual fluorescence of the dinucleotide in the static fluorescence spectrum.

Ultrafast electron transport across nano gaps in nanowire circuits

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

Potma, Eric O.

In this Program we aim for a closer look at electron transfer through single molecules. To achieve this, we use ultrafast laser pulses to time stamp an electron tunneling event in a molecule that is connected between two metallic electrodes, while reading out the electron current. A key aspect of this project is the use of metallic substrates with plasmonic activity to efficiently manipulate the tunneling probability. The first Phase of this program is concerned with developing highly sensitive tools for the ultrafast optical manipulation of tethered molecules through the evanescent surface field of plasmonic substrates. The second Phase ofmore » the program aims to use these tools for exercising control over the electron tunneling probability.« less

Optical Amplification of Spin Noise Spectroscopy via Homodyne Detection

NASA Astrophysics Data System (ADS)

Sterin, Pavel; Wiegand, Julia; Hübner, Jens; Oestreich, Michael

2018-03-01

Spin noise (SN) spectroscopy measurements on delicate semiconductor spin systems, like single (In,Ga)As quantum dots, are currently not limited by optical shot noise but rather by the electronic noise of the detection system. We report on a realization of homodyne SN spectroscopy enabling shot-noise-limited SN measurements. The proof-of-principle measurements on impurities in an isotopically enriched rubidium atom vapor show that homodyne SN spectroscopy can be utilized even in the low-frequency spectrum, which facilitates advanced semiconductor spin research like higher order SN measurements on spin qubits.

Demonstration of Berry Phase in Optical Spectroscopy

NASA Technical Reports Server (NTRS)

Xia, Hui-Rong; Zhang, Yong; Jiang, Hong-Ji; Ding, Liang-En

1996-01-01

In this paper we demonstrate that the observed phase shift of the RF signal and its intensity dependence under extreme low pump and probe laser field conditions are dominated by Berry phase effect in optical spectroscopy with good adiabatic approximation, which provides all features' agreements between the theoretical and the experimental results.

An ultrafast electron microscope gun driven by two-photon photoemission from a nanotip cathode

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

Bormann, Reiner; Strauch, Stefanie; Schäfer, Sascha, E-mail: schaefer@ph4.physik.uni-goettingen.de

We experimentally and numerically investigate the performance of an advanced ultrafast electron source, based on two-photon photoemission from a tungsten needle cathode incorporated in an electron microscope gun geometry. Emission properties are characterized as a function of the electrostatic gun settings, and operating conditions leading to laser-triggered electron beams of very low emittance (below 20 nm mrad) are identified. The results highlight the excellent suitability of optically driven nano-cathodes for the further development of ultrafast transmission electron microscopy.

Precision Spectroscopy, Diode Lasers, and Optical Frequency Measurement Technology

NASA Technical Reports Server (NTRS)

Hollberg, Leo (Editor); Fox, Richard (Editor); Waltman, Steve (Editor); Robinson, Hugh

1998-01-01

This compilation is a selected set of reprints from the Optical Frequency Measurement Group of the Time and Frequency Division of the National Institute of Standards and Technology, and consists of work published between 1987 and 1997. The two main programs represented here are (1) development of tunable diode-laser technology for scientific applications and precision measurements, and (2) research toward the goal of realizing optical-frequency measurements and synthesis. The papers are organized chronologically in five, somewhat arbitrarily chosen categories: Diode Laser Technology, Tunable Laser Systems, Laser Spectroscopy, Optical Synthesis and Extended Wavelength Coverage, and Multi-Photon Interactions and Optical Coherences.

Developing a structure-function model for the cryptophyte phycoerythrin 545 using ultrahigh resolution crystallography and ultrafast laser spectroscopy.

PubMed

Doust, Alexander B; Marai, Christopher N J; Harrop, Stephen J; Wilk, Krystyna E; Curmi, Paul M G; Scholes, Gregory D

2004-11-12

Cryptophyte algae differ from cyanobacteria and red algae in the architecture of their photosynthetic light harvesting systems, even though all three are evolutionarily related. Central to cryptophyte light harvesting is the soluble antenna protein phycoerythrin 545 (PE545). The ultrahigh resolution crystal structure of PE545, isolated from a unicellular cryptophyte Rhodomonas CS24, is reported at both 1.1A and 0.97A resolution, revealing details of the conformation and environments of the chromophores. Absorption, emission and polarized steady state spectroscopy (298K, 77K), as well as ultrafast (20fs time resolution) measurements of population dynamics are reported. Coupled with complementary quantum chemical calculations of electronic transitions of the bilins, these enable assignment of spectral absorption characteristics to each chromophore in the structure. Spectral differences between the tetrapyrrole pigments due to chemical differences between bilins, as well as their binding and interaction with the local protein environment are described. Based on these assignments, and considering customized optical properties such as strong coupling, a model for light harvesting by PE545 is developed which explains the fast, directional harvesting of excitation energy. The excitation energy is funnelled from four peripheral pigments (beta158,beta82) into a central chromophore dimer (beta50/beta61) in approximately 1ps. Those chromophores, in turn, transfer the excitation energy to the red absorbing molecules located at the periphery of the complex in approximately 4ps. A final resonance energy transfer step sensitizes just one of the alpha19 bilins on a time scale of 22ps. Furthermore, it is concluded that binding of PE545 to the thylakoid membrane is not essential for efficient energy transfer to the integral membrane chlorophyll a-containing complexes associated with PS-II.

Overview of selected seminal optical science and photonics processes in nature

NASA Astrophysics Data System (ADS)

Alfano, Robert R.

2016-03-01

This presentation gives an overview on some of seminal research in optical science, condensed matter physics, biophysics, biology, biomedical, nonlinear optics, and structure light propagation and interactions at CCNY and GTE Labs over past 46 years. The advent of ultrafast laser pulses with picosecond and femtosecond pulses and optical spectroscopy (label free native fluorescence and Raman) has led to unravel some of mysteries in the molecular world leading to breakthroughs in various areas of science and medicine. The following topics are discussed: white light continuum called now Supercontinuum (SC); first direct measurement of Optical Phonon's lifetimes; first observation of creation of daughter vibrations in time from excited mother vibration in liquids; first direct measurement of creation and decay of Spin Angular Momentum of electrons in GaAs where picosecond Circular Polarized Light carrying Optical Spin Angular Momentum is generated; Pulse break up into ballistic, snake and diffusive components in scattering media such as um beads and tissues; and use of optical spectroscopy for first cancer detection in label free tissues. Most recently, advances in Biomedical Optics showed that Tryptophan as a key biomarker for aggressive cancers; there are three new optical windows with the Golden window #3 the best for penetrating tissue from 1600 nm to 1800 nm; Complex light with OAM offers potential deeper tissue penetration and Resonance Raman excited using magic 532 nm wavelength in tissues.

Optical phantoms with variable properties and geometries for diffuse and fluorescence optical spectroscopy

NASA Astrophysics Data System (ADS)

Leh, Barbara; Siebert, Rainer; Hamzeh, Hussein; Menard, Laurent; Duval, Marie-Alix; Charon, Yves; Abi Haidar, Darine

2012-10-01

Growing interest in optical instruments for biomedical applications has increased the use of optically calibrated phantoms. Often associated with tissue modeling, phantoms allow the characterization of optical devices for clinical purposes. Fluorescent gel phantoms have been developed, mimicking optical properties of healthy and tumorous brain tissues. Specific geometries of dedicated molds offer multiple-layer phantoms with variable thicknesses and monolayer phantoms with cylindrical inclusions at various depths and diameters. Organic chromophores are added to allow fluorescence spectroscopy. These phantoms are designed to be used with 405 nm as the excitation wavelength. This wavelength is then adapted to excite large endogenous molecules. The benefits of these phantoms in understanding fluorescence tissue analysis are then demonstrated. In particular, detectability aspects as a function of geometrical and optical parameters are presented and discussed.

Ultrafast studies of organometallic photochemistry: The mechanism of carbon-hydrogen bond activation in solution

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

Bromberg, S.E.

1998-05-01

When certain organometallic compounds are photoexcited in room temperature alkane solution, they are able to break or activate the C-H bonds of the solvent. Understanding this potentially practical reaction requires a detailed knowledge of the entire reaction mechanism. Because of the dynamic nature of chemical reactions, time-resolved spectroscopy is commonly employed to follow the important events that take place as reactants are converted to products. For the organometallic reactions examined here, the electronic/structural characteristics of the chemical systems along with the time scales for the key steps in the reaction make ultrafast UV/Vis and IR spectroscopy along with nanosecond Step-Scanmore » FTIR spectroscopy the ideal techniques to use for this study. An initial study of the photophysics of (non-activating) model metal carbonyls centering on the photodissociation of M(CO){sub 6} (M = Cr, W, Mo) was carried out in alkane solutions using ultrafast IR spectroscopy. Next, picosecond UV/vis studies of the C-H bond activation reaction of Cp{sup *}M(CO){sub 2} (M = Rh, Ir), conducted in room temperature alkane solution, are described in an effort to investigate the origin of the low quantum yield for bond cleavage ({approximately}1%). To monitor the chemistry that takes place in the reaction after CO is lost, a system with higher quantum yield is required. The reaction of Tp{sup *}Rh(CO){sub 2} (Tp{sup *} = HB-Pz{sub 3}{sup *}, Pz{sup *} = 3,5-dimethylpyrazolyl) in alkanes has a quantum yield of {approximately}30%, making time resolved spectroscopic measurements possible. From ultrafast IR experiments, two subsequently formed intermediates were observed. The nature of these intermediates are discussed and the first comprehensive reaction mechanism for a photochemical C-H activating organometallic complex is presented.« less

Dual-modal cancer detection based on optical pH sensing and Raman spectroscopy

NASA Astrophysics Data System (ADS)

Kim, Soogeun; Lee, Seung Ho; Min, Sun Young; Byun, Kyung Min; Lee, Soo Yeol

2017-10-01

A dual-modal approach using Raman spectroscopy and optical pH sensing was investigated to discriminate between normal and cancerous tissues. Raman spectroscopy has demonstrated the potential for in vivo cancer detection. However, Raman spectroscopy has suffered from strong fluorescence background of biological samples and subtle spectral differences between normal and disease tissues. To overcome those issues, pH sensing is adopted to Raman spectroscopy as a dual-modal approach. Based on the fact that the pH level in cancerous tissues is lower than that in normal tissues due to insufficient vasculature formation, the dual-modal approach combining the chemical information of Raman spectrum and the metabolic information of pH level can improve the specificity of cancer diagnosis. From human breast tissue samples, Raman spectra and pH levels are measured using fiber-optic-based Raman and pH probes, respectively. The pH sensing is based on the dependence of pH level on optical transmission spectrum. Multivariate statistical analysis is performed to evaluate the classification capability of the dual-modal method. The analytical results show that the dual-modal method based on Raman spectroscopy and optical pH sensing can improve the performance of cancer classification.

In vivo determination of multiple indices of periodontal inflammation by optical spectroscopy

PubMed Central

Liu, KZ; Xiang, XM; Man, A; Sowa, MG; Cholakis, N; Ghiabi, E; Singer, DL; Scott, DA

2008-01-01

Background and Objective Visible – near infrared (optical) spectroscopy can be used to measure regional tissue hemodynamics and edema and, therefore, may represent an ideal tool with which to non-invasively study periodontal inflammation. The study objective was to evaluate the ability of optical spectroscopy to simultaneously determine multiple inflammatory indices (tissue oxygenation, total tissue hemoglobin, deoxyhemoglobin, oxygenated hemoglobin, and tissue edema) in periodontal tissues in vivo. Material and Methods Spectra were obtained, processed, and evaluated from healthy, gingivitis, and periodontitis sites (n = 133) using a portable optical – near infrared spectrometer. A modified Beer-Lambert unmixing model that incorporates a nonparametric scattering loss function was used to determine the relative contribution of each inflammatory component to the overall spectrum. Results Optical spectroscopy was harnessed to successfully generate complex inflammatory profiles in periodontal tissues. Tissue oxygenation at periodontitis sites was significantly decreased (p<0.05) compared to gingivitis and healthy controls. This is largely due to an increase in deoxyhemoglobin in the periodontitis sites compared to healthy (p<0.01) and gingivitis (p=0.05) sites. Tissue water content per se showed no significant difference between the sites but a water index associated with tissue electrolyte levels and temperature differed was significantly between periodontitis sites when compared to both healthy and gingivitis sites (p<0.03). Conclusion This study establishes that optical spectroscopy can simultaneously determine multiple inflammatory indices directly in the periodontal tissues in vivo. Visible - near infrared spectroscopy has the potential to be developed into a simple, reagent-free, user friendly, chair-side, site-specific, diagnostic and prognostic test for periodontitis. PMID:18973538

Ultrafast far-infrared studies of vanadates &mdash Multiple routes for an insulator to metal transition

NASA Astrophysics Data System (ADS)

Liu, Mengkun

The metal insulator transition in vanadates has been studied for decades and yet new discoveries still spring up revealing new physics, especially among two of the most studied members: Vanadium sesquioxide (V20 3) and Vanadium dioxide (VO2). Although subtleties abound, both of the materials have first order insulator to metal phase transitions that are considered to be related to strong electron-electron (e-e) correlation. Further, ultrafast spectroscopy of strongly correlated materials has generated great interest in the field given the potential to dynamically distinguish the difference between electronic (spin) response versus lattice responses due to the associated characteristic energy and time scales. In this thesis, I mainly focus on utilizing ultrafast optical and THz spectroscopy to study phase transition dynamics in high quality V20 3 and VO2 thin films epitaxially grown on different substrates. The main findings of the thesis are: (1) Despite the fact that the insulator to metal transition (IMT) in V203 is electron-correlation driven, lattice distortion plays an important role. Coherent oscillations in the far-infrared conductivity are observed resulting from coherent acoustic phonon modulation of the bandwidth W. The same order of lattice distortion induces less of an effect on the electron transport in VO2 in comparison to V203. This is directly related to the difference in latent heat of the phase transitions in VO2 and V203. (2) It is possible for the IMT to occur with very little structural change in epitaxial strained VO2 films, like in the case of Cr doped or strained V203. However, in V02, this necessitates a large strain which is only possible by clamping to a substrate with larger c axis parameter through epitaxial growth. This is demonstrated for VO 2 films on TiO2 substrates. (3) Initiating an ultrafast photo-induced insulator-to-metal transition (IMT) is not only possible with above bandgap excitation, but also possible with high-field far

Ultrafast carrier dynamics in bilayer graphene studied by broadband infrared pump-probe spectroscopy

NASA Astrophysics Data System (ADS)

Limmer, Thomas; da Como, Enrico; Niggebaum, Alexander; Feldmann, Jochen

2010-03-01

Recently, bilayer graphene gained a large interest because of its electrically tunable gap appearing in the middle infrared part of the electromagnetic spectrum. This feature is expected to open a number of applications of bilayer graphene in optoelectronics. In this communication we report on the first pump-probe experiment on a single bilayer flake with an unprecedented probe photon energy interval (0.25 -- 1.3 eV). Single flakes were prepared by mechanical exfoliation of graphite and transferred to calcium fluoride substrates. When illuminated with 800 nm (1.5 eV) pump pulses the induced change in transmission shows an ultrafast saturation of the interband transitions from 1.3 to 0.5 eV. In this energy range the saturation recovery occurs within 3 ps and is consistent with an ultrafast relaxation of hot carriers. Interestingly, we report on the observation of a resonance at 0.4 eV characterized by a longer dynamics. The results are discussed considering many-body interactions.

Optical Spectroscopy of New Materials

NASA Technical Reports Server (NTRS)

White, Susan M.; Arnold, James O. (Technical Monitor)

1993-01-01

Composites are currently used for a rapidly expanding number of applications including aircraft structures, rocket nozzles, thermal protection of spacecraft, high performance ablative surfaces, sports equipment including skis, tennis rackets and bicycles, lightweight automobile components, cutting tools, and optical-grade mirrors. Composites are formed from two or more insoluble materials to produce a material with superior properties to either component. Composites range from dispersion-hardened alloys to advanced fiber-reinforced composites. UV/VIS and FTIR spectroscopy currently is used to evaluate the bonding between the matrix and the fibers, monitor the curing process of a polymer, measure surface contamination, characterize the interphase material, monitor anion transport in polymer phases, characterize the void formation (voids must be minimized because, like cracks in a bulk material, they lead to failure), characterize the surface of the fiber component, and measure the overall optical properties for energy balances.

Temperature dependence of the hydrated electron's excited-state relaxation. II. Elucidating the relaxation mechanism through ultrafast transient absorption and stimulated emission spectroscopy

NASA Astrophysics Data System (ADS)

Farr, Erik P.; Zho, Chen-Chen; Challa, Jagannadha R.; Schwartz, Benjamin J.

2017-08-01

The structure of the hydrated electron, particularly whether it exists primarily within a cavity or encompasses interior water molecules, has been the subject of much recent debate. In Paper I [C.-C. Zho et al., J. Chem. Phys. 147, 074503 (2017)], we found that mixed quantum/classical simulations with cavity and non-cavity pseudopotentials gave different predictions for the temperature dependence of the rate of the photoexcited hydrated electron's relaxation back to the ground state. In this paper, we measure the ultrafast transient absorption spectroscopy of the photoexcited hydrated electron as a function of temperature to confront the predictions of our simulations. The ultrafast spectroscopy clearly shows faster relaxation dynamics at higher temperatures. In particular, the transient absorption data show a clear excess bleach beyond that of the equilibrium hydrated electron's ground-state absorption that can only be explained by stimulated emission. This stimulated emission component, which is consistent with the experimentally known fluorescence spectrum of the hydrated electron, decreases in both amplitude and lifetime as the temperature is increased. We use a kinetic model to globally fit the temperature-dependent transient absorption data at multiple temperatures ranging from 0 to 45 °C. We find the room-temperature lifetime of the excited-state hydrated electron to be 137 ±40 fs, in close agreement with recent time-resolved photoelectron spectroscopy (TRPES) experiments and in strong support of the "non-adiabatic" picture of the hydrated electron's excited-state relaxation. Moreover, we find that the excited-state lifetime is strongly temperature dependent, changing by slightly more than a factor of two over the 45 °C temperature range explored. This temperature dependence of the lifetime, along with a faster rate of ground-state cooling with increasing bulk temperature, should be directly observable by future TRPES experiments. Our data also suggest

Nonlinear Optical Spectroscopy of Two-Dimensional Materials

NASA Astrophysics Data System (ADS)

Cui, Qiannan

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

Mitigating intrinsic defects and laser damage using pulsetrain-burst (>100 MHz) ultrafast laser processing

NASA Astrophysics Data System (ADS)

McKinney, Luke; Frank, Felix; Graper, David; Dean, Jesse; Forrester, Paul; Rioblanc, Maxence; Nantel, Marc; Marjoribanks, Robin

2005-09-01

Ultrafast-laser micromachining has promise as an approach to trimming and 'healing' small laser-produced damage sites in laser-system optics--a common experience in state-of-the-art high-power laser systems. More-conventional approaches currently include mechanical micromachining, chemical modification, and treatment using cw and long-pulse lasers. Laser-optics materials of interest include fused silica, multilayer dielectric stacks for anti-reflection coatings or high-reflectivity mirrors, and inorganic crystals such as KD*P, used for Pockels cells and frequency-doubling. We report on novel efforts using ultrafast-laser pulsetrain-burst processing (microsecond bursts at 133 MHz) to mitigate damage in fused silica, dielectric coatings, and KD*P crystals. We have established the characteristics of pulsetrain-burst micromachining in fused silica, multilayer mirrors, and KD*P, and determined the etch rates and morphology under different conditions of fluence-delivery. From all of these, we have begun to identify new means to optimize the laser-repair of optics defects and damage.

Optical Spectroscopy for Noninvasive Monitoring of Stem Cell Differentiation

PubMed Central

Downes, Andrew; Mouras, Rabah; Elfick, Alistair

2010-01-01

There is a requirement for a noninvasive technique to monitor stem cell differentiation. Several candidates based on optical spectroscopy are discussed in this review: Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, and coherent anti-Stokes Raman scattering (CARS) microscopy. These techniques are briefly described, and the ability of each to distinguish undifferentiated from differentiated cells is discussed. FTIR spectroscopy has demonstrated its ability to distinguish between stem cells and their derivatives. Raman spectroscopy shows a clear reduction in DNA and RNA concentrations during embryonic stem cell differentiation (agreeing with the well-known reduction in the nucleus to cytoplasm ratio) and also shows clear increases in mineral content during differentiation of mesenchymal stem cells. CARS microscopy can map these DNA, RNA, and mineral concentrations at high speed, and Mutliplex CARS spectroscopy/microscopy is highlighted as the technique with most promise for future applications. PMID:20182537

Longitudinal evaluation of patients with oral potentially malignant disorders using optical imaging and spectroscopy

NASA Astrophysics Data System (ADS)

Schwarz, Richard A.; Pierce, Mark C.; Mondrik, Sharon; Gao, Wen; Quinn, Mary K.; Bhattar, Vijayashree; Williams, Michelle D.; Vigneswaran, Nadarajah; Gillenwater, Ann M.; Richards-Kortum, Rebecca

2012-02-01

Dysplastic and cancerous alterations in oral tissue can be detected noninvasively in vivo using optical techniques including autofluorescence imaging, high-resolution imaging, and spectroscopy. Interim results are presented from a longitudinal study in which optical imaging and spectroscopy were used to evaluate the progression of lesions over time in patients at high risk for development of oral cancer. Over 100 patients with oral potentially malignant disorders have been enrolled in the study to date. Areas of concern in the oral cavity are measured using widefield autofluorescence imaging and depth-sensitive optical spectroscopy during successive clinical visits. Autofluorescence intensity patterns and autofluorescence spectra are tracked over time and correlated with clinical observations. Patients whose lesions progress and who undergo surgery are also measured in the operating room immediately prior to surgery using autofluorescence imaging and spectroscopy, with the addition of intraoperative high-resolution imaging to characterize nuclear size, nuclear crowding, and tissue architecture at selected sites. Optical measurements are compared to histopathology results from biopsies and surgical specimens collected from the measured sites. Autofluorescence imaging and spectroscopy measurements are continued during post-surgery followup visits. We examined correlations between clinical impression and optical classification over time with an average followup period of 4 months. The data collected to date suggest that multimodal optical techniques may aid in noninvasive monitoring of the progression of oral premalignant lesions, biopsy site selection, and accurate delineation of lesion extent during surgery.

Mapping momentum-dependent electron-phonon coupling and nonequilibrium phonon dynamics with ultrafast electron diffuse scattering

NASA Astrophysics Data System (ADS)

Stern, Mark J.; René de Cotret, Laurent P.; Otto, Martin R.; Chatelain, Robert P.; Boisvert, Jean-Philippe; Sutton, Mark; Siwick, Bradley J.

2018-04-01

Despite their fundamental role in determining material properties, detailed momentum-dependent information on the strength of electron-phonon and phonon-phonon coupling (EPC and PPC, respectively) across the entire Brillouin zone has remained elusive. Here we demonstrate that ultrafast electron diffuse scattering (UEDS) directly provides such information. By exploiting symmetry-based selection rules and time resolution, scattering from different phonon branches can be distinguished even without energy resolution. Using graphite as a model system, we show that UEDS patterns map the relative EPC and PPC strength through their profound sensitivity to photoinduced changes in phonon populations. We measure strong EPC to the K -point TO phonon of A1' symmetry (K -A1' ) and along the entire TO branch between Γ -K , not only to the Γ -E2 g phonon. We also determine that the subsequent phonon relaxation of these strongly coupled optical phonons involve three stages: decay via several identifiable channels to TA and LA phonons (1 -2 ps), intraband thermalization of the non-equilibrium TA/LA phonon populations (30 -40 ps) and interband relaxation of the TA/LA modes (115 ps). Combining UEDS with ultrafast angle-resolved photoelectron spectroscopy will yield a complete picture of the dynamics within and between electron and phonon subsystems, helping to unravel complex phases in which the intertwined nature of these systems has a strong influence on emergent properties.

Exploring Ultrafast Structural Dynamics for Energetic Enhancement or Disruption

DTIC Science & Technology

2016-03-01

it. In a pump -push/ dump probe experiment, a secondary laser pulse (push/ dump ) is used after the initial perturbation due to the pump pulse. The...increased. The pump -push/ dump probe technique is a difficult experiment that requires a highly stable laser source. Ultrafast pump -probe experiments...decomposition of solids. Journal of Applied Physics. 2001;89:4156–4166. 17. Kee TW. Femtosecond pump -push-probe and pump - dump -probe spectroscopy of

Optical tuning of electronic valleys (Conference Presentation)

NASA Astrophysics Data System (ADS)

Sie, Edbert J.; Gedik, Nuh

2017-02-01

Monolayer transition-metal dichalcogenides such as MoS2 and WS2 are prime examples of atomically thin semiconducting crystals that exhibit remarkable electronic and optical properties. They have a pair of valleys that can serve as a new electronic degree of freedom, and these valleys obey optical selection rules with circularly polarized light. Here, we discuss how ultrafast laser pulses can be used to tune their energy levels in a controllable valley-selective manner. The energy tunability is extremely large, comparable to what would be obtained using a hundred Tesla of magnetic field. We will also show that such valley tunability can be performed while we effectively manipulate the valley selection rules. Finally, we will explore the prospect of using this technique through photoemission spectroscopy to create a new phase of matter called a valley Floquet topological insulator.

Correlating structural dynamics and catalytic activity of AgAu nanoparticles with ultrafast spectroscopy and all-atom molecular dynamics simulations.

PubMed

Ferbonink, G F; Rodrigues, T S; Dos Santos, D P; Camargo, P H C; Albuquerque, R Q; Nome, R A

2018-05-29

In this study, we investigated hollow AgAu nanoparticles with the goal of improving our understanding of the composition-dependent catalytic activity of these nanoparticles. AgAu nanoparticles were synthesized via the galvanic replacement method with controlled size and nanoparticle compositions. We studied extinction spectra with UV-Vis spectroscopy and simulations based on Mie theory and the boundary element method, and ultrafast spectroscopy measurements to characterize decay constants and the overall energy transfer dynamics as a function of AgAu composition. Electron-phonon coupling times for each composition were obtained from pump-power dependent pump-probe transients. These spectroscopic studies showed how nanoscale surface segregation, hollow interiors and porosity affect the surface plasmon resonance wavelength and fundamental electron-phonon coupling times. Analysis of the spectroscopic data was used to correlate electron-phonon coupling times to AgAu composition, and thus to surface segregation and catalytic activity. We have performed all-atom molecular dynamics simulations of model hollow AgAu core-shell nanoparticles to characterize nanoparticle stability and equilibrium structures, besides providing atomic level views of nanoparticle surface segregation. Overall, the basic atomistic and electron-lattice dynamics of core-shell AgAu nanoparticles characterized here thus aid the mechanistic understanding and performance optimization of AgAu nanoparticle catalysts.

Distinctive Spectral Features of Exciton and Excimer States in the Ultrafast Electronic Deactivation of the Adenine Dinucleotide

NASA Astrophysics Data System (ADS)

Stuhldreier, Mayra C.; Röttger, Katharina; Temps, Friedrich

We report the observation by transient absorption spectroscopy of distinctive spectro-temporal signatures of delocalized exciton versus relaxed, weakly bound excimer states in the ultrafast electronic deactivation after UV photoexcitation of the adenine dinucleotide.

Gold-Based Nanostructures for Ultrafast Dynamic Nanothermometer

NASA Astrophysics Data System (ADS)

Sun, Hongtao

Nano-scale temperature measurements are of significance for fundamental understanding of functional applications and nanosystems, requiring ultimate miniaturization of thermometers with reduced size, maintained sensitivity, simplicity and accuracy of temperature reading. Particularly, grand challenges exist for scenarios of combustion or thermal shock where materials may be subjected to drastic temperature variations and extreme thermal flux, and dynamic thermal sensors with an ultrafast response (seconds to milliseconds) are yet to be developed. Targeting the developments of advanced nano-scale thermal sensors with a fast time response and rapid readout, this thesis reports innovative designs of high surface-to-volume ratio gold nanostructures including ultrathin gold island films on transparent quartz substrates and silica-gold core-shell (SiO2 Au) nanospheres as potential dynamic thermal sensors for accurate temperature determination. The sensing mechanism is based on strong temperature dependences of the thermally-dewetting-induced morphological self-reorganization and characteristic surface plasmon (SP) absorption of the gold nanostructures. The irreversible thermally-induced morphological and optical signatures behave as characteristic "fingerprints" for temperature recording, allowing the retrieval of thermal history ex-situ. The fundamental studies of thermal-induced dewetting process and its corresponding unique optical properties were extensively investigated by high resolution scanning electron microscopy (HR-SEM), atomic force microscopy (AFM), and UV-vis-NIR spectroscopy, which illustrate temperature and time dependent variations. As compared with current nanothermometer technologies such as metal-filled nanotubes, our thermo-sensor offers positively synergistic advantages of ultrafast time response, permanent recording and fast readout of thermal history, and ex-situ capability for effective temperature measurements. In addition, SiO2 Au nanospheres

Ultrafast Pulse Generation in an Organic Nanoparticle-Array Laser.

PubMed

Daskalakis, Konstantinos S; Väkeväinen, Aaro I; Martikainen, Jani-Petri; Hakala, Tommi K; Törmä, Päivi

2018-04-11

Nanoscale coherent light sources offer potentially ultrafast modulation speeds, which could be utilized for novel sensors and optical switches. Plasmonic periodic structures combined with organic gain materials have emerged as promising candidates for such nanolasers. Their plasmonic component provides high intensity and ultrafast nanoscale-confined electric fields, while organic gain materials offer fabrication flexibility and a low acquisition cost. Despite reports on lasing in plasmonic arrays, lasing dynamics in these structures have not been experimentally studied yet. Here we demonstrate, for the first time, an organic dye nanoparticle-array laser with more than a 100 GHz modulation bandwidth. We show that the lasing modulation speed can be tuned by the array parameters. Accelerated dynamics is observed for plasmonic lasing modes at the blue side of the dye emission.

Free-electron laser spectroscopy in biology, medicine, and materials science; Proceedings of the Meeting, Los Angeles, CA, Jan. 22, 1993

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

Schwettman, H.A.

1993-01-01

Various papers on FEL spectroscopy in biology, medicine, and materials science are presented. Individual topics addressed include: Vanderbilt University FEL Center, FIR FEL facility at the University of California/Santa Barbara, FEL research facilities and opportunities at Duke, facilities at the Stanford Picosecond FEL Center, FIR nonlinear response of electrons in semiconductor nanostructures, FIR harmonic generation from semiconductor heterostructures, intrinsic response times of double-barrier resonant tunneling diodes at tetrahertz frequencies, semiconductor spectroscopy and ablation processes with the Vanderbilt FEL. Also discussed are: picosecond nonlinear optics in semiconductor quantum wells with the SCA FEL, excitation spectroscopy of thin-film disordered semiconductors, biophysical applicationmore » of FELs, FEL investigation of energy transfer in condensed phase systems, probing protein photochemistry and dynamics with ultrafast infrared spectroscopy, plasma ablation of hard tissues by FEL, FEL irradiation of the cornea.« less

Single-electron pulses for ultrafast diffraction

PubMed Central

Aidelsburger, M.; Kirchner, F. O.; Krausz, F.; Baum, P.

2010-01-01

Visualization of atomic-scale structural motion by ultrafast electron diffraction and microscopy requires electron packets of shortest duration and highest coherence. We report on the generation and application of single-electron pulses for this purpose. Photoelectric emission from metal surfaces is studied with tunable ultraviolet pulses in the femtosecond regime. The bandwidth, efficiency, coherence, and electron pulse duration are investigated in dependence on excitation wavelength, intensity, and laser bandwidth. At photon energies close to the cathode’s work function, the electron pulse duration shortens significantly and approaches a threshold that is determined by interplay of the optical pulse width and the acceleration field. An optimized choice of laser wavelength and bandwidth results in sub-100-fs electron pulses. We demonstrate single-electron diffraction from polycrystalline diamond films and reveal the favorable influences of matched photon energies on the coherence volume of single-electron wave packets. We discuss the consequences of our findings for the physics of the photoelectric effect and for applications of single-electron pulses in ultrafast 4D imaging of structural dynamics. PMID:21041681

Temperature-dependence of hypersound dynamics in SrTiO3/SrRuO3 heterostructures studied by ultrafast spectroscopy

NASA Astrophysics Data System (ADS)

Yang, Chi-Yuan; Yadav, Ajay K.; Ramesh, Ramamoorthy; Wen, Yu-Chieh; Hsu, Chia-Hao; Wu, Maw-Kuen; Chia, Chih-Ta; Lin, Kung-Hsuan

Strontium titanate (SrTiO3, STO) and strontium ruthenate (SrRuO3, SRO) are complex oxide with perovskite structure. Their property, such as thermoelectricity and superconductivity, has been widely investigated for scientific and industrial purposes. Recently, complex oxide heterostructures can be grown by pulsed laser deposition. It opens many possibilities f or new properties of materials. With ultrafast pump-probe spectroscopy, we demonstrated that metal-like SRO thin film can be served as a phonon transducer to generate hypersound with frequency of several tens to several hundreads of GHz. This technique can be utilized to study not only the elastic properties of perovskite thin films but also the interfaces. In this study, we used this technique to study the temperature dependence of structural phases in STO. During the crossing over the soft-mode transition in STO around 110 K, the shortening of phonon lifetime were also observed.

Ultrafast transmission electron microscopy using a laser-driven field emitter: Femtosecond resolution with a high coherence electron beam.

PubMed

Feist, Armin; Bach, Nora; Rubiano da Silva, Nara; Danz, Thomas; Möller, Marcel; Priebe, Katharina E; Domröse, Till; Gatzmann, J Gregor; Rost, Stefan; Schauss, Jakob; Strauch, Stefanie; Bormann, Reiner; Sivis, Murat; Schäfer, Sascha; Ropers, Claus

2017-05-01

We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the Göttingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in ultrafast electron microscopy of 9Å focused beam diameter, 200fs pulse duration and 0.6eV energy width. We illustrate the possibility to conduct ultrafast imaging, diffraction, holography and spectroscopy with this instrument and also discuss opportunities to harness quantum coherent interactions between intense laser fields and free-electron beams. Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.

Rippling ultrafast dynamics of suspended 2D monolayers, graphene

PubMed Central

Hu, Jianbo; Vanacore, Giovanni M.; Cepellotti, Andrea; Marzari, Nicola; Zewail, Ahmed H.

2016-01-01

Here, using ultrafast electron crystallography (UEC), we report the observation of rippling dynamics in suspended monolayer graphene, the prototypical and most-studied 2D material. The high scattering cross-section for electron/matter interaction, the atomic-scale spatial resolution, and the ultrafast temporal resolution of UEC represent the key elements that make this technique a unique tool for the dynamic investigation of 2D materials, and nanostructures in general. We find that, at early time after the ultrafast optical excitation, graphene undergoes a lattice expansion on a time scale of 5 ps, which is due to the excitation of short-wavelength in-plane acoustic phonon modes that stretch the graphene plane. On a longer time scale, a slower thermal contraction with a time constant of 50 ps is observed and associated with the excitation of out-of-plane phonon modes, which drive the lattice toward thermal equilibrium with the well-known negative thermal expansion coefficient of graphene. From our results and first-principles lattice dynamics and out-of-equilibrium relaxation calculations, we quantitatively elucidate the deformation dynamics of the graphene unit cell. PMID:27791028

Effectively Single-Mode Self-Recovering Ultrafast Nonlinear Nanowire Surface Plasmons

NASA Astrophysics Data System (ADS)

Tuniz, Alessandro; Weidlich, Stefan; Schmidt, Markus A.

2018-04-01

We report on a regime for surface-plasmon propagation, which is robust to defects and effectively single mode, and we exploit it for accessing the ultrafast nonlinear response of gold on centimeter-long subwavelength-diameter cylindrical nanowires. The hybrid plasmonic-photonic platform is formed by a gold nanowire, monolithically integrated into the core of an optical fiber. We show that, despite the dual-waveguide nature of this structure, the long-range surface plasmon is the only effectively propagating mode in the near infrared, which self-recovers in the presence of gaps via a light-recapturing effect. This self-recovery overcomes detrimental effects of wire discontinuities and enables measurements of the ultrafast nonlinearity of gold, which we perform for a 28-fs pulse duration.

Optical trapping and Raman spectroscopy of solid particles.

PubMed

Rkiouak, L; Tang, M J; Camp, J C J; McGregor, J; Watson, I M; Cox, R A; Kalberer, M; Ward, A D; Pope, F D

2014-06-21

The heterogeneous interactions of gas molecules on solid particles are crucial in many areas of science, engineering and technology. Such interactions play a critical role in atmospheric chemistry and in heterogeneous catalysis, a key technology in the energy and chemical industries. Investigating heterogeneous interactions upon single levitated particles can provide significant insight into these important processes. Various methodologies exist for levitating micron sized particles including: optical, electrical and acoustic techniques. Prior to this study, the optical levitation of solid micron scale particles has proved difficult to achieve over timescales relevant to the above applications. In this work, a new vertically configured counter propagating dual beam optical trap was optimized to levitate a range of solid particles in air. Silica (SiO2), α-alumina (Al2O3), titania (TiO2) and polystyrene were stably trapped with a high trapping efficiency (Q = 0.42). The longest stable trapping experiment was conducted continuously for 24 hours, and there are no obvious constraints on trapping time beyond this period. Therefore, the methodology described in this paper should be of major benefit to various research communities. The strength of the new technique is demonstrated by the simultaneous levitation and spectroscopic interrogation of silica particles by Raman spectroscopy. In particular, the adsorption of water upon silica was investigated under controlled relative humidity environments. Furthermore, the collision and coagulation behaviour of silica particles with microdroplets of sulphuric acid was followed using both optical imaging and Raman spectroscopy.

Ultrafast Carrier dynamics of InxGa1-xN nanostructures grown directly on Si(111)

NASA Astrophysics Data System (ADS)

Kumar, Praveen; Devi, Pooja; Rodriguez⁠, P. E. D. S.; Kumar, Manish; Shivling, V. D.; Noetzel, Richard; Sharma, Chhavi; Sinha, R. K.; Kumar, Mahesh

2018-05-01

We show a flux dependence changes in structural, optical and electronic properties of InxGa1-xN nanostructures (NSs) namely nanocolumns (NCs), nanoflakes (NFs) and nanowall network (NWN) grown directly on Si(111) surface. Field emission scanning electron microscopy (FESEM) images were recorded to see morphological changes from NFs to NCs and NWNc etc, while high-resolution X-ray diffraction (HRXRD) ω-2θ scans were used to determine In incorporation. The maximum In incorporation was observed to be 20, 33 and 38% for the sharp transition from NFs to NCs and NWNs, respectively. The charge carrier dynamics of these grown NSs were probed using Ultrafast Femtosecond Transient Absorption Spectroscopy (UFTAS) with excitation at 350 nm pump wavelength. The UFTAS studies show the comparative charge carriers dynamics of the NWS, NCs and NFs. The charge carrier studies show a higher lifetime in NWNs as compare to NCs and NFs. Further, to examine electronic structure and level of degeneracy of these NSs, core-level and valence band spectra were analyzed by X-ray photoelectron spectroscopy (XPS), which manifest the upward band bending ranging from 0.2 eV to 0.4 eV.

Engine throat/nozzle optics for plume spectroscopy

NASA Technical Reports Server (NTRS)

Bickford, R. L.; Duncan, D. B.

1991-01-01

The Task 2.0 Engine Throat/Nozzle Optics for Plume Spectroscopy, effort was performed under the NASA LeRC Development of Life Prediction Capabilities for Liquid Propellant Rocket Engines program. This Task produced the engineering design of an optical probe to enable spectroscopic measurements within the SSME main chamber. The probe mounts on the SSME nozzle aft manifold and collects light emitted from the throat plane and chamber. Light collected by the probe is transferred to a spectrometer through a fiber optic cable. The design analyses indicate that the probe will function throughout the engine operating cycle and is suitable for both test stand and flight operations. By detecting metallic emissions that are indicative of component degradation or incipient failure, engine shutdown can be initiated before catastrophic failure. This capability will protect valuable test stand hardware and provide enhanced mission safety.

Time-domain separation of optical properties from structural transitions in resonantly bonded materials.

PubMed

Waldecker, Lutz; Miller, Timothy A; Rudé, Miquel; Bertoni, Roman; Osmond, Johann; Pruneri, Valerio; Simpson, Robert E; Ernstorfer, Ralph; Wall, Simon

2015-10-01

The extreme electro-optical contrast between crystalline and amorphous states in phase-change materials is routinely exploited in optical data storage and future applications include universal memories, flexible displays, reconfigurable optical circuits, and logic devices. Optical contrast is believed to arise owing to a change in crystallinity. Here we show that the connection between optical properties and structure can be broken. Using a combination of single-shot femtosecond electron diffraction and optical spectroscopy, we simultaneously follow the lattice dynamics and dielectric function in the phase-change material Ge2Sb2Te5 during an irreversible state transformation. The dielectric function changes by 30% within 100 fs owing to a rapid depletion of electrons from resonantly bonded states. This occurs without perturbing the crystallinity of the lattice, which heats with a 2-ps time constant. The optical changes are an order of magnitude larger than those achievable with silicon and present new routes to manipulate light on an ultrafast timescale without structural changes.

Study of blast event propagation in different media using a novel ultrafast miniature optical pressure sensor

NASA Astrophysics Data System (ADS)

Zou, Xiaotian; Wu, Nan; Tian, Ye; Zhang, Hongtao; Niezrecki, Christopher; Wang, Xingwei

2011-06-01

Traumatic brain injury (TBI, also called intracranial injury) is a high potential threat to our soldiers. A helmet structural health monitoring system can be effectively used to study the effects of ballistic/blast events on the helmet and human skull to prevent soldiers from TBI. However, one of the biggest challenges lies in that the pressure sensor installed inside the helmet system must be fast enough to capture the blast wave during the transient period. In this paper, an ultrafast optical fiber sensor is presented to measure the blast signal. The sensor is based on a Fabry-Pérot (FP) interferometeric principle. An FP cavity is built between the endface of an etched optical fiber tip and the silica thin diaphragm attached on the end of a multimode optical fiber. The sensor is small enough to be installed in different locations of a helmet to measure blast pressure simultaneously. Several groups of tests regarding multi-layer blast events were conducted to evaluate the sensors' performance. The sensors were mounted in different segments of a shock tube side by side with the reference sensors, to measure a rapidly increasing pressure. The segments of the shock tube were filled with different media. The results demonstrated that our sensors' responses agreed well with those from the electrical reference sensors. In addition, the home-made shock tube could provide a good resource to study the propagation of blast event in different media.

Fast responses from slowly relaxing'' liquids: A comparative study of the femtosecond dynamics of triacetin, ethylene glycol, and water

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

Chang, Y.J.; Castner, E.W. Jr.

1993-11-15

We have measured the ultrafast solvent relaxation of liquid ethylene glycol, triacetin, and water by means of femtosecond polarization spectroscopy, using optical-heterodyne-detected Raman-induced Kerr-effect spectroscopy. In the viscous liquids triacetin and ethylene glycol, femtosecond relaxation processes were resolved. Not surprisingly, the femtosecond nonlinear optical response of ethylene glycol is quite similar to that of water. Using the theory of Maroncelli, Kumar, and Papazyan, we transform the pure-nuclear solvent response into a dipolar-solvation correlation function for comparison with ultrafast electron-transfer reaction rates.

Fast responses from ``slowly relaxing'' liquids: A comparative study of the femtosecond dynamics of triacetin, ethylene glycol, and water

NASA Astrophysics Data System (ADS)

Chang, Yong Joon; Castner, Edward W., Jr.

1993-11-01

We have measured the ultrafast solvent relaxation of liquid ethylene glycol, triacetin, and water by means of femtosecond polarization spectroscopy, using optical-heterodyne-detected Raman-induced Kerr-effect spectroscopy. In the viscous liquids triacetin and ethylene glycol, femtosecond relaxation processes were resolved. Not surprisingly, the femtosecond nonlinear optical response of ethylene glycol is quite similar to that of water. Using the theory of Maroncelli, Kumar, and Papazyan, we transform the pure-nuclear solvent response into a dipolar-solvation correlation function for comparison with ultrafast electron-transfer reaction rates.

Microresonator-Based Optical Frequency Combs: A Time Domain Perspective

DTIC Science & Technology

2016-04-19

optics; ultrafast optics 16. SECURITY CLASSIFICATION OF: 17. LIMITATION OF ABSTRACT 18. NUMBER OF PAGES 19a. NAME OF RESPONSIBLE PERSON a...generation at frequency spacings down to 25 GHz, in the range where convenient electronic detection is possible. (c) Our best Purdue microrings had...time domain measurements of the generated combs, leading to observation of novel, ultrafast dark pulse waveforms, have introduced new structures such

Magneto-optical spectroscopy of Co{sub 2}FeSi Heusler compound

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

Veis, M., E-mail: veis@karlov.mff.cuni.cz; Beran, L.; Antos, R.

2014-05-07

Magneto-optical and electronic properties of the Co{sub 2}FeSi Heusler compound were studied by polar Kerr magneto-optical spectroscopy and ab-initio calculations. The thin-film samples were grown by dc/rf magnetron co-sputtering on MgO(100) substrates. A Cr seed layer was deposited prior to the Co{sub 2}FeSi layer to achieve its epitaxial growth. The magneto-optical spectroscopy was carried out using generalized magneto-optical ellipsometry with rotating analyzer in the photon energy range from 1.4 to 5.5 eV with an applied magnetic field of up to 1.2 T. The polar Kerr spectra showed a smooth spectral behavior up to 5.5 eV indicating nearly free charge carriers. Experimental data weremore » compared with ab-initio calculations based on density functional theory employing the full-potential linearized augmented plane wave method.« less

Ultrafast acousto-plasmonics in gold nanoparticle superlattices

NASA Astrophysics Data System (ADS)

Ruello, P.; Ayouch, A.; Vaudel, G.; Pezeril, T.; Delorme, N.; Sato, S.; Kimura, K.; Gusev, V. E.

2015-11-01

We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticle superlattices (NPSs). The experiments have been performed with an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow us to estimate first the fundamental mechanical parameters such as the collective elastic response (sound velocity) of the NPS and the nanocontact elastic stiffness. Furthermore, it appears that the light-induced coherent acoustic-phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly four times the optical skin depth in gold. The modeling of the transient optical reflectivity indicates that the mechanism of phonons generation is achieved through ultrafast heating of the NPS assisted by light excitation of the volume plasmon polariton. Based on these results, we demonstrate that it is possible to map the photon-electron-phonon interaction in subwavelength nanostructures which, in particular, provides insights on the fundamental properties of these nanometamaterials.

Hydrogen Bond Switching among Flavin and Amino Acid Side Chains in the BLUF Photoreceptor Observed by Ultrafast Infrared Spectroscopy

PubMed Central

Bonetti, Cosimo; Mathes, Tilo; van Stokkum, Ivo H. M.; Mullen, Katharine M.; Groot, Marie-Louise; van Grondelle, Rienk; Hegemann, Peter; Kennis, John T. M.

2008-01-01

BLUF domains constitute a recently discovered class of photoreceptor proteins found in bacteria and eukaryotic algae. BLUF domains are blue-light sensitive through a FAD cofactor that is involved in an extensive hydrogen-bond network with nearby amino acid side chains, including a highly conserved tyrosine and glutamine. The participation of particular amino acid side chains in the ultrafast hydrogen-bond switching reaction with FAD that underlies photoactivation of BLUF domains is assessed by means of ultrafast infrared spectroscopy. Blue-light absorption by FAD results in formation of FAD•− and a bleach of the tyrosine ring vibrational mode on a picosecond timescale, showing that electron transfer from tyrosine to FAD constitutes the primary photochemistry. This interpretation is supported by the absence of a kinetic isotope effect on the fluorescence decay on H/D exchange. Subsequent protonation of FAD•− to result in FADH• on a picosecond timescale is evidenced by the appearance of a N-H bending mode at the FAD N5 protonation site and of a FADH• C=N stretch marker mode, with tyrosine as the likely proton donor. FADH• is reoxidized in 67 ps (180 ps in D2O) to result in a long-lived hydrogen-bond switched network around FAD. This hydrogen-bond switch shows infrared signatures from the C-OH stretch of tyrosine and the FAD C4=O and C=N stretches, which indicate increased hydrogen-bond strength at all these sites. The results support a previously hypothesized rotation of glutamine by ∼180° through a light-driven radical-pair mechanism as the determinant of the hydrogen-bond switch. PMID:18708458

Use of interfacial layers to prolong hole lifetimes in hematite probed by ultrafast transient absorption spectroscopy

NASA Astrophysics Data System (ADS)

Paradzah, Alexander T.; Diale, Mmantsae; Maabong, Kelebogile; Krüger, Tjaart P. J.

2018-04-01

Hematite is a widely investigated material for applications in solar water oxidation due primarily to its small bandgap. However, full realization of the material continues to be hampered by fast electron-hole recombination rates among other weaknesses such as low hole mobility, short hole diffusion length and low conductivity. To address the problem of fast electron-hole recombination, researchers have resorted to growth of nano-structured hematite, doping and use of under-layers. Under-layer materials enhance the photo-current by minimising electron-hole recombination through suppressing of back electron flow from the substrate, such as fluorine-doped tin oxide (FTO), to hematite. We have carried out ultrafast transient absorption spectroscopy on hematite in which Nb2O5 and SnO2 materials were used as interfacial layers to enhance hole lifetimes. The transient absorption data was fit with four different lifetimes ranging from a few hundred femtoseconds to a few nanoseconds. We show that the electron-hole recombination is slower in samples where interfacial layers are used than in pristine hematite. We also develop a model through target analysis to illustrate the effect of under-layers on electron-hole recombination rates in hematite thin films.

Two-dimensional infrared spectroscopy of intermolecular hydrogen bonds in the condensed phase.

PubMed

Elsaesser, Thomas

2009-09-15

Hydrogen bonding plays a key role in the structural, physical, and chemical properties of liquids such as water and in macromolecular structures such as proteins. Vibrational spectroscopy is an important tool for understanding hydrogen bonding because it provides a way to observe local molecular geometries and their interaction with the environment. Linear vibrational spectroscopy has mapped characteristic changes of vibrational spectra and the occurrence of new bands that form upon hydrogen bonding. However, linear vibrational spectroscopy gives very limited insight into ultrafast dynamics of the underlying molecular interactions, such as the motions of hydrogen-bonded groups, energy dissipation and delocalization, and the fluctuations within hydrogen-bonded structures that occur in the ultrafast time domain. Nonlinear vibrational spectroscopy with its femtosecond time resolution can discern these dynamic processes in real time and has emerged as an important tool for unraveling molecular dynamics and for quantifying interactions that govern the vibrational and structural dynamics of hydrogen bonds. This Account reviews recent progress originating from third-order nonlinear methods of coherent multidimensional vibrational spectroscopy. Ultrafast dynamics of intermolecular hydrogen bonds are addressed for a number of prototype systems: hydrogen-bonded carboxylic acid dimers in an aprotic liquid environment, the disordered fluctuating hydrogen-bond network of liquid water, and DNA oligomers interacting with water. Cyclic carboxylic acid dimers display a rich scheme of vibrational couplings, resulting in OH stretching absorption bands with highly complex spectral envelopes. Two-dimensional spectroscopy of acetic acid dimers in a nonpolar liquid environment demonstrates that multiple Fermi resonances of the OH stretching mode with overtones and combination tones of fingerprint vibrations dominate both the 2D and linear absorption spectra. The coupling of the OH

Remote in-situ laser-induced breakdown spectroscopy using optical fibers

NASA Astrophysics Data System (ADS)

Marquardt, Brian James

The following dissertation describes the development of methods for performing remote Laser-Induced Breakdown Spectroscopy (LIBS) using optical fibers. Studies were performed to determine the optimal excitation and collection parameters for remote LIBS measurements of glasses, soils and paint. A number of fiber-optic LIBS probes were developed and used to characterize various samples by plasma emission spectroscopy. A novel method for launching high-power laser pulses into optical fibers without causing catastrophic failure is introduced. A systematic study of a number of commercially available optical fibers was performed to determine which optical fibers were best suited for delivering high-power laser pulses. The general design of an all fiber-optic LIBS probe is described and applied to the determination of Pb in soil. A fiber-optic probe was developed for the microanalysis of solid samples remotely by LIBS, Raman spectroscopy and Raman imaging. The design of the probe allows for real-time sample imaging in-situ using coherent imaging fibers. This allows for precise atomic emission and Raman measurements to be performed remotely on samples in hostile or inaccessible environments. A novel technique was developed for collecting spectral plasma images using an acousto-optic tunable filter (AOTF). The spatial and temporal characteristics of the plasma were studied as a function of delay time. From the plasma images the distribution of Pb emission could be determined and fiber-optic designs could be optimized for signal collection. The performance of a two fiber LIBS probe is demonstrated for the determination of the amount of lead in samples of dry paint. It is shown that dry paint samples can be analyzed for their Pb content in-situ using a fiber-optic LIBS probe with detection limits well below the levels currently regulated by the Consumer Products Safety Commission. It is also shown that these measurements can be performed on both latex and enamel paints, and

Scanning, non-contact, hybrid broadband diffuse optical spectroscopy and diffuse correlation spectroscopy system.

PubMed

Johansson, Johannes D; Mireles, Miguel; Morales-Dalmau, Jordi; Farzam, Parisa; Martínez-Lozano, Mar; Casanovas, Oriol; Durduran, Turgut

2016-02-01

A scanning system for small animal imaging using non-contact, hybrid broadband diffuse optical spectroscopy (ncDOS) and diffuse correlation spectroscopy (ncDCS) is presented. The ncDOS uses a two-dimensional spectrophotometer retrieving broadband (610-900 nm) spectral information from up to fifty-seven source-detector distances between 2 and 5 mm. The ncDCS data is simultaneously acquired from four source-detector pairs. The sample is scanned in two dimensions while tracking variations in height. The system has been validated with liquid phantoms, demonstrated in vivo on a human fingertip during an arm cuff occlusion and on a group of mice with xenoimplanted renal cell carcinoma.

Auger electron spectroscopy, secondary ion mass spectroscopy and optical characterization of a-C-H and BN films

NASA Technical Reports Server (NTRS)

Pouch, J. J.; Alterovitz, S. A.; Warner, J. D.

1986-01-01

The amorphous dielectrics a-C:H and BN were deposited on III-V semiconductors. Optical band gaps as high as 3 eV were measured for a-C:H generated by C4H10 plasmas; a comparison was made with bad gaps obtained from films prepared by CH4 glow discharges. The ion beam deposited BN films exhibited amorphous behavior with band gaps on the order of 5 eV. Film compositions were studied by Auger electron spectroscopy (AES), x-ray photoelectron spectroscopy (XPS) and secondary ion mass spectrometry (SIMS). The optical properties were characterized by ellipsometry, UV/VIS absorption, and IR reflection and transmission. Etching rates of a-C:H subjected to O2 dicharges were determined.

Effects of environmental conditions on the ultrafast carrier dynamics in graphene revealed by terahertz spectroscopy

NASA Astrophysics Data System (ADS)

Hafez, H. A.; Chai, X.; Sekine, Y.; Takamura, M.; Oguri, K.; Al-Naib, I.; Dignam, M. M.; Hibino, H.; Ozaki, T.

2017-04-01

A thorough understanding of the stability of graphene under ambient environmental conditions is essential for future graphene-based applications. In this paper, we study the effects of ambient temperature on the properties of monolayer graphene using terahertz time-domain spectroscopy as well as time-resolved terahertz spectroscopy enabled by an optical-pump/terahertz-probe technique. The observations show that graphene is extremely sensitive to the ambient environmental conditions and behaves differently depending on the sample preparation technique and the initial Fermi level. The analysis of the spectroscopic data is supported by van der Pauw and Hall effect measurements of the carrier mobility and carrier density at temperatures comparable to those tested in our THz spectroscopic experiments.

Realizing high-quality ultralarge momentum states and ultrafast topological transitions using semiconductor hyperbolic metamaterials

DOE PAGES