Three-Dimensional Self-Organization in Nanocomposite Layered Systems by Ultrafast Laser Pulses.

PubMed

Liu, Zeming; Siegel, Jan; Garcia-Lechuga, Mario; Epicier, Thierry; Lefkir, Yaya; Reynaud, Stéphanie; Bugnet, Matthieu; Vocanson, Francis; Solis, Javier; Vitrant, Guy; Destouches, Nathalie

2017-05-23

Controlling plasmonic systems with nanometer resolution in transparent films and their colors over large nonplanar areas is a key issue for spreading their use in various industrial fields. Using light to direct self-organization mechanisms provides high-speed and flexible processes to meet this challenge. Here, we describe a route for the laser-induced self-organization of metallic nanostructures in 3D. Going beyond the production of planar nanopatterns, we demonstrate that ultrafast laser-induced excitation combined with nonlinear feedback mechanisms in a nanocomposite thin film can lead to 3D self-organized nanostructured films. The process, which can be extended to complex layered composite systems, produces highly uniform large-area nanopatterns. We show that 3D self-organization originates from the simultaneous excitation of independent optical modes at different depths in the film and is activated by the plasmon-induced charge separation and thermally induced NP growth mechanisms. This laser color marking technique enables multiplexed optical image encoding and the generated nanostructured Ag NPs:TiO 2 films offer great promise for applications in solar energy harvesting, photocatalysis, or photochromic devices.

Phase transformation pathways of Ln2O3 irradiated by ultrafast laser

NASA Astrophysics Data System (ADS)

Rittman, Dylan; Solomon, Jonathan; Chen, Curtis; Tracy, Cameron; Yalisove, Steven; Asta, Mark; Mao, Wendy; Ewing, Rodney

Ultrafast laser irradiation induces highly non-equilibrium conditions in materials through intense electronic excitation over very short timescales. Here, we show that ultrafast laser irradiation drives an irreversible cubic-to-monoclinic phase transformation in Ln2O3 (Ln = Er-Lu). A combination of grazing incidence X-ray diffraction and transmission electron microscopy is used to characterize the amount and depth-dependence of the phase transformation. Results indicate that-although all materials experience the same transformation-it is achieved through different damage mechanisms (pressure vs. thermal), and the short timescales associated with damage provides non-equilibrium routes of material modification. Ab initio molecular dynamics are used to isolate the effects of electronic excitations, and results are shown to be consistent with the trend in radiation resistance observed experimentally. Overall, this study provides a path to gain insight into the relationship between a material's equilibrium phase diagram and its behavior under highly non-equilibrium conditions. DOE/BES.

4D imaging of transient structures and morphologies in ultrafast electron microscopy.

PubMed

Barwick, Brett; Park, Hyun Soon; Kwon, Oh-Hoon; Baskin, J Spencer; Zewail, Ahmed H

2008-11-21

With advances in spatial resolution reaching the atomic scale, two-dimensional (2D) and 3D imaging in electron microscopy has become an essential methodology in various fields of study. Here, we report 4D imaging, with in situ spatiotemporal resolutions, in ultrafast electron microscopy (UEM). The ability to capture selected-area-image dynamics with pixel resolution and to control the time separation between pulses for temporal cooling of the specimen made possible studies of fleeting structures and morphologies. We demonstrate the potential for applications with two examples, gold and graphite. For gold, after thermally induced stress, we determined the atomic structural expansion, the nonthermal lattice temperature, and the ultrafast transients of warping/bulging. In contrast, in graphite, striking coherent transients of the structure were observed in both image and diffraction, directly measuring, on the nanoscale, the longitudinal resonance period governed by Young's elastic modulus. The success of these studies demonstrates the promise of UEM in real-space imaging of dynamics.

Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements.

PubMed

Heilpern, Tal; Manjare, Manoj; Govorov, Alexander O; Wiederrecht, Gary P; Gray, Stephen K; Harutyunyan, Hayk

2018-05-10

Developing a fundamental understanding of ultrafast non-thermal processes in metallic nanosystems will lead to applications in photodetection, photochemistry and photonic circuitry. Typically, non-thermal and thermal carrier populations in plasmonic systems are inferred either by making assumptions about the functional form of the initial energy distribution or using indirect sensors like localized plasmon frequency shifts. Here we directly determine non-thermal and thermal distributions and dynamics in thin films by applying a double inversion procedure to optical pump-probe data that relates the reflectivity changes around Fermi energy to the changes in the dielectric function and in the single-electron energy band occupancies. When applied to normal incidence measurements our method uncovers the ultrafast excitation of a non-Fermi-Dirac distribution and its subsequent thermalization dynamics. Furthermore, when applied to the Kretschmann configuration, we show that the excitation of propagating plasmons leads to a broader energy distribution of electrons due to the enhanced Landau damping.

Two-magnon bound state causes ultrafast thermally induced magnetisation switching

PubMed Central

Barker, J.; Atxitia, U.; Ostler, T. A.; Hovorka, O.; Chubykalo-Fesenko, O.; Chantrell, R. W.

2013-01-01

There has been much interest recently in the discovery of thermally induced magnetisation switching using femtosecond laser excitation, where a ferrimagnetic system can be switched deterministically without an applied magnetic field. Experimental results suggest that the reversal occurs due to intrinsic material properties, but so far the microscopic mechanism responsible for reversal has not been identified. Using computational and analytic methods we show that the switching is caused by the excitation of two-magnon bound states, the properties of which are dependent on material factors. This discovery allows us to accurately predict the onset of switching and the identification of this mechanism will allow new classes of materials to be identified or designed for memory devices in the THz regime. PMID:24253110

Ultrafast photo-induced hidden phases in strained manganite thin films

NASA Astrophysics Data System (ADS)

Zhang, Jingdi; McLeod, A. S.; Zhang, Gu-Feng; Stoica, Vladimir; Jin, Feng; Gu, Mingqiang; Gopalan, Venkatraman; Freeland, John W.; Wu, Wenbin; Rondinelli, James; Wen, Haidan; Basov, D. N.; Averitt, R. D.

Correlated transition metal oxides (TMOs) are particularly sensitive to external control because of energy degeneracy in a complex energy landscape that promote a plethora of metastable states. However, it remains a grand challenge to actively control and fully explore the rich landscape of TMOs. Dynamic control with pulsed photons can overcome energetic barriers, enabling access to transient or metastable states that are not thermally accessible. In the past, we have demonstrated that mode-selective single-laser-pulse excitation of a strained manganite thin film La2/3Ca1/3MnO3 initiates a persistent phase transition from an emergent antiferromagnetic insulating ground state to a ferromagnetic metallic metastable state. Beyond the photo-induced insulator to metal transition, we recently discovered a new peculiar photo-induced hidden phase, identified by an experimental approach that combines ultrafast pump-probe spectroscopy, THz spectroscopy, X-ray diffraction, cryogenic near-field spectroscopy and SHG probe. This work is funded by the DOE, Office of Science, Office of Basic Energy Science under Award Numbers DE-SC0012375 and DE-SC0012592.

Effect of Carrier Thermalization Dynamics on Light Emission and Amplification in Organometal Halide Perovskites.

PubMed

Chen, Kai; Barker, Alex J; Morgan, Francis L C; Halpert, Jonathan E; Hodgkiss, Justin M

2015-01-02

The remarkable rise of organometal halide perovskites as solar photovoltaic materials has been followed by promising developments in light-emitting devices, including lasers. Here we present unique insights into the processes leading to photon emission in these materials. We employ ultrafast broadband photoluminescence (PL) and transient absorption spectroscopies to directly link density dependent ultrafast charge dynamics to PL. We find that exceptionally strong PL at the band edge is preceded by thermalization of free charge carriers. Short-lived PL above the band gap is clear evidence of nonexcitonic emission from hot carriers, and ultrafast PL depolarization confirms that uncorrelated charge pairs are precursors to photon emission. Carrier thermalization has a profound effect on amplified stimulated emission at high fluence; the delayed onset of optical gain we resolve within the first 10 ps and the unusual oscillatory behavior are both consequences of the kinetic interplay between carrier thermalization and optical gain.

Thermal Conductivity of a Nanoscale Yttrium Iron Garnet Thin-Film Prepared by the Sol-Gel Process

PubMed Central

2017-01-01

The thermal conductivity of a nanoscale yttrium iron garnet (Y3Fe5O12, YIG) thin-film prepared by a sol-gel method was evaluated using the ultrafast pump-probe technique in the present study. The thermoreflectance change on the surface of a 250 nm thick YIG film, induced by the irradiation of femtosecond laser pulses, was measured, and curve fitting of a numerical solution for the transient heat conduction equation to the experimental data was performed using the finite difference method in order to extract the thermal property. Results show that the film’s thermal conductivity is 22–83% higher than the properties of bulk YIG materials prepared by different fabrication techniques, reflecting the microstructural characteristics and quality of the film. PMID:28858249

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

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.

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 studies of shock induced chemistry-scaling down the size by turning up the heat

NASA Astrophysics Data System (ADS)

McGrane, Shawn

2015-06-01

We will discuss recent progress in measuring time dependent shock induced chemistry on picosecond time scales. Data on the shock induced chemistry of liquids observed through picosecond interferometric and spectroscopic measurements will be reconciled with shock induced chemistry observed on orders of magnitude larger time and length scales from plate impact experiments reported in the literature. While some materials exhibit chemistry consistent with simple thermal models, other materials, like nitromethane, seem to have more complex behavior. More detailed measurements of chemistry and temperature across a broad range of shock conditions, and therefore time and length scales, will be needed to achieve a real understanding of shock induced chemistry, and we will discuss efforts and opportunities in this direction.

Cooperative inter- and intra-layer lattice dynamics of photoexcited multi-walled carbon nanotubes studied by ultrafast electron diffraction.

PubMed

Sun, Shuaishuai; Li, Zhongwen; Li, Zi-An; Xiao, Ruijuan; Zhang, Ming; Tian, Huanfang; Yang, Huaixin; Li, Jianqi

2018-04-26

Optical tuning and probing ultrafast structural response of nanomaterials driven by electronic excitation constitute a challenging but promising approach for understanding microscopic mechanisms and applications in microelectromechanical systems and optoelectrical devices. Here we use pulsed electron diffraction in a transmission electron microscope to investigate laser-induced tubular lattice dynamics of multi-walled carbon nanotubes (MWCNTs) with varying laser fluence and initial specimen temperature. Our photoexcitation experiments demonstrate cooperative and inverse collective atomic motions in intralayer and interlayer directions, whose strengths and rates depend on pump fluence. The electron-driven and thermally driven structural responses with opposite amplitudes cause a crossover between intralayer and interlayer directions. Our ab initio calculations support these findings and reveal that electrons excited from π to π* orbitals in a carbon tube weaken the intralayer bonds while strengthening the interlayer bonds along the radial direction. Moreover, by probing the structural dynamics of MWCNTs at initial temperatures of 300 and 100 K, we uncover the concomitance of thermal and nonthermal dynamical processes and their mutual influence in MWCNTs. Our results illustrate the nature of electron-driven nonthermal process and electron-phonon thermalization in the MWCNTs, and bear implications for the intricate energy conversion and transfer in materials at the nanoscale.

Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4.

PubMed

Dean, M P M; Cao, Y; Liu, X; Wall, S; Zhu, D; Mankowsky, R; Thampy, V; Chen, X M; Vale, J G; Casa, D; Kim, Jungho; Said, A H; Juhas, P; Alonso-Mori, R; Glownia, J M; Robert, A; Robinson, J; Sikorski, M; Song, S; Kozina, M; Lemke, H; Patthey, L; Owada, S; Katayama, T; Yabashi, M; Tanaka, Yoshikazu; Togashi, T; Liu, J; Rayan Serrao, C; Kim, B J; Huber, L; Chang, C-L; McMorrow, D F; Först, M; Hill, J P

2016-06-01

Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity. Recently, photo-excitation has been used to induce similarly exotic states transiently. However, the lack of available probes of magnetic correlations in the time domain hinders our understanding of these photo-induced states and how they could be controlled. Here, we implement magnetic resonant inelastic X-ray scattering at a free-electron laser to directly determine the magnetic dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state, 2 ps after the excitation, exhibits strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. These two-dimensional (2D) in-plane Néel correlations recover within a few picoseconds, whereas the three-dimensional (3D) long-range magnetic order restores on a fluence-dependent timescale of a few hundred picoseconds. The marked difference in these two timescales implies that the dimensionality of magnetic correlations is vital for our understanding of ultrafast magnetic dynamics.

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

Substrate thermal conductivity controls the ability to manufacture microstructures via laser-induced direct write

NASA Astrophysics Data System (ADS)

Tomko, John A.; Olson, David H.; Braun, Jeffrey L.; Kelliher, Andrew P.; Kaehr, Bryan; Hopkins, Patrick E.

2018-01-01

In controlling the thermal properties of the surrounding environment, we provide insight into the underlying mechanisms driving the widely used laser direct write method for additive manufacturing. We find that the onset of silver nitrate reduction for the formation of direct write structures directly corresponds to the calculated steady-state temperature rises associated with both continuous wave and high-repetition rate, ultrafast pulsed laser systems. Furthermore, varying the geometry of the heat affected zone, which is controllable based on in-plane thermal diffusion in the substrate, and laser power, allows for control of the written geometries without any prior substrate preparation. These findings allow for the advance of rapid manufacturing of micro- and nanoscale structures with minimal material constraints through consideration of the laser-controllable thermal transport in ionic liquid/substrate media.

Ultrafast demagnetization at high temperatures

NASA Astrophysics Data System (ADS)

Hoveyda, F.; Hohenstein, E.; Judge, R.; Smadici, S.

2018-05-01

Time-resolved pump-probe measurements were made at variable heat accumulation in Co/Pd superlattices. Heat accumulation increases the baseline temperature and decreases the equilibrium magnetization. Transient ultrafast demagnetization first develops with higher fluence in parallel with strong equilibrium thermal spin fluctuations. The ultrafast demagnetization is then gradually removed as the equilibrium temperature approaches the Curie temperature. The transient magnetization time-dependence is well fit with the spin-flip scattering model.

Imaging Spatial Variations in the Dissipation and Transport of Thermal Energy within Individual Silicon Nanowires Using Ultrafast Microscopy.

PubMed

Cating, Emma E M; Pinion, Christopher W; Van Goethem, Erika M; Gabriel, Michelle M; Cahoon, James F; Papanikolas, John M

2016-01-13

Thermal management is an important consideration for most nanoelectronic devices, and an understanding of the thermal conductivity of individual device components is critical for the design of thermally efficient systems. However, it can be difficult to directly probe local changes in thermal conductivity within a nanoscale system. Here, we utilize the time-resolved and diffraction-limited imaging capabilities of ultrafast pump-probe microscopy to determine, in a contact-free configuration, the local thermal conductivity in individual Si nanowires (NWs). By suspending single NWs across microfabricated trenches in a quartz substrate, the properties of the same NW both on and off the substrate are directly compared. We find the substrate has no effect on the recombination lifetime or diffusion length of photogenerated charge carriers; however, it significantly impacts the thermal relaxation properties of the NW. In substrate-supported regions, thermal energy deposited into the lattice by the ultrafast laser pulse dissipates within ∼10 ns through thermal diffusion and coupling to the substrate. In suspended regions, the thermal energy persists for over 100 ns, and we directly image the time-resolved spatial motion of the thermal signal. Quantitative analysis of the transient images permits direct determination of the NW's local thermal conductivity, which we find to be a factor of ∼4 smaller than in bulk Si. Our results point to the strong potential of pump-probe microscopy to be used as an all-optical method to quantify the effects of localized environment and morphology on the thermal transport characteristics of individual nanostructured components.

Modelling ultrafast laser ablation

NASA Astrophysics Data System (ADS)

Rethfeld, Baerbel; Ivanov, Dmitriy S.; E Garcia, Martin; Anisimov, Sergei I.

2017-05-01

This review is devoted to the study of ultrafast laser ablation of solids and liquids. The ablation of condensed matter under exposure to subpicosecond laser pulses has a number of peculiar properties which distinguish this process from ablation induced by nanosecond and longer laser pulses. The process of ultrafast ablation includes light absorption by electrons in the skin layer, energy transfer from the skin layer to target interior by nonlinear electronic heat conduction, relaxation of the electron and ion temperatures, ultrafast melting, hydrodynamic expansion of heated matter accompanied by the formation of metastable states and subsequent formation of breaks in condensed matter. In case of ultrashort laser excitation, these processes are temporally separated and can thus be studied separately. As for energy absorption, we consider peculiarities of the case of metal irradiation in contrast to dielectrics and semiconductors. We discuss the energy dissipation processes of electronic thermal wave and lattice heating. Different types of phase transitions after ultrashort laser pulse irradiation as melting, vaporization or transitions to warm dense matter are discussed. Also nonthermal phase transitions, directly caused by the electronic excitation before considerable lattice heating, are considered. The final material removal occurs from the physical point of view as expansion of heated matter; here we discuss approaches of hydrodynamics, as well as molecular dynamic simulations directly following the atomic movements. Hybrid approaches tracing the dynamics of excited electrons, energy dissipation and structural dynamics in a combined simulation are reviewed as well.

Beating Darwin-Bragg losses in lab-based ultrafast x-ray experiments

PubMed Central

Fullagar, Wilfred K.; Uhlig, Jens; Mandal, Ujjwal; Kurunthu, Dharmalingam; El Nahhas, Amal; Tatsuno, Hideyuki; Honarfar, Alireza; Parnefjord Gustafsson, Fredrik; Sundström, Villy; Palosaari, Mikko R. J.; Kinnunen, Kimmo M.; Maasilta, Ilari J.; Miaja-Avila, Luis; O'Neil, Galen C.; Joe, Young Il; Swetz, Daniel S.; Ullom, Joel N.

2017-01-01

The use of low temperature thermal detectors for avoiding Darwin-Bragg losses in lab-based ultrafast experiments has begun. An outline of the background of this new development is offered, showing the relevant history and initiative taken by this work. PMID:28396880

Plasmonic nanostructure assisted HHG in NIR spectrum and thermal analysis

NASA Astrophysics Data System (ADS)

Ebadian, H.; Mohebbi, M.

2018-02-01

We study plasmonic nanoparticle assisted high-order harmonic generation (HHG), illuminated by near infrared (NIR) laser sources, and the effect of the geometry of some different dimers on HHG cutoff frequency is evaluated. Dimers are installed on different dielectric substrates and the electric field enhancement factors are simulated. We demonstrate that NIR femto-fiber sources are good options for the HHG process. Such sources can induce significant inhomogeneous electric fields in the nanogaps; and consequently, high harmonic cutoff orders more than 250 will be obtained. Moreover, by time dependent thermal analysis of Au nanoparticles exposed to NIR ultrafast high power lasers, we could determine the temperature distribution in the nanoparticle and substrate.

Ultrafast Shock Compression Hugoniot Data of beta-CL-20 and TATB Thin Films

NASA Astrophysics Data System (ADS)

Zaug, Joseph; Armstrong, Michael; Grivickas, Paulius; Tappan, Alexander; Kohl, Ian; Rodriguez, Mark; Knepper, Robert; Crowhurst, Jonathan; Stavrou, Elissaios; Bastea, Sorin

2017-06-01

The shock induced initiation threshold of two energetic materials, CL-20 and TATB are remarkably different; CL-20 is a relatively shock sensitive energetic material and TATB is considered an insensitive high explosive (IHE). Here we report ultrafast laser-based shockwave hydrodynamic data on the 100 ps timescale with 10 ps time resolution to further develop density dependent unreacted shock Hugoniot equations of state (UEOS) and to elucidate ultrafast timescale shock initiation processes for these two vastly different HEs. Thin film samples were made by vacuum thermal evaporation of the explosive on a deposited aluminum ablator layer. The deposited explosives were characterized by scanning electron microscopy, surface profilometry, and x-ray diffraction. Our preliminary UEOS results (up range of 1.3 - 1.8 km/s) from shock compressed beta-CL-20 agree reasonably well with extrapolated pseudo-velocities computed from epsilon-CL-20 isothermal diamond-anvil cell EOS measurements. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344. Sandia National Laboratories is a multi-mission laboratory managed and operated by Sandia Corporati.

Substrate thermal conductivity controls the ability to manufacture microstructures via laser-induced direct write

DOE PAGES

Tomko, John A.; Olson, David H.; Braun, Jeffrey L.; ...

2018-01-30

In controlling the thermal properties of the surrounding environment, we provide insight into the underlying mechanisms driving the widely used laser direct write method for additive manufacturing. In this study, we find that the onset of silver nitrate reduction for the formation of direct write structures directly corresponds to the calculated steady-state temperature rises associated with both continuous wave and high-repetition rate, ultrafast pulsed laser systems. Furthermore, varying the geometry of the heat affected zone, which is controllable based on in-plane thermal diffusion in the substrate, and laser power, allows for control of the written geometries without any prior substratemore » preparation. In conclusion, these findings allow for the advance of rapid manufacturing of micro- and nanoscale structures with minimal material constraints through consideration of the laser-controllable thermal transport in ionic liquid/substrate media.« less

Substrate thermal conductivity controls the ability to manufacture microstructures via laser-induced direct write

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

Tomko, John A.; Olson, David H.; Braun, Jeffrey L.

In controlling the thermal properties of the surrounding environment, we provide insight into the underlying mechanisms driving the widely used laser direct write method for additive manufacturing. In this study, we find that the onset of silver nitrate reduction for the formation of direct write structures directly corresponds to the calculated steady-state temperature rises associated with both continuous wave and high-repetition rate, ultrafast pulsed laser systems. Furthermore, varying the geometry of the heat affected zone, which is controllable based on in-plane thermal diffusion in the substrate, and laser power, allows for control of the written geometries without any prior substratemore » preparation. In conclusion, these findings allow for the advance of rapid manufacturing of micro- and nanoscale structures with minimal material constraints through consideration of the laser-controllable thermal transport in ionic liquid/substrate media.« 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.

Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr 2IrO 4

DOE PAGES

Dean, M. P. M.; Cao, Y.; Liu, X.; ...

2016-05-09

Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity 1, 2, 3, 4. Recently, photo-excitation has been used to induce similarly exotic states transiently 5, 6, 7. However, the lack of available probes of magnetic correlations in the time domain hinders our understanding of these photo-induced states and how they could be controlled. Here, we implement magnetic resonant inelastic X-ray scattering at a free-electron laser to directly determine the magnetic dynamics after photo-doping the Mott insulator Sr 2IrO 4. We find that the non-equilibrium state, 2more » ps after the excitation, exhibits strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. These two-dimensional (2D) in-plane Néel correlations recover within a few picoseconds, whereas the three-dimensional (3D) long-range magnetic order restores on a fluence-dependent timescale of a few hundred picoseconds. In conclusion, the marked difference in these two timescales implies that the dimensionality of magnetic correlations is vital for our understanding of ultrafast magnetic dynamics.« less

Ultrafast demagnetization by hot electrons: Diffusion or super-diffusion?

PubMed

Salvatella, G; Gort, R; Bühlmann, K; Däster, S; Vaterlaus, A; Acremann, Y

2016-09-01

Ultrafast demagnetization of ferromagnetic metals can be achieved by a heat pulse propagating in the electron gas of a non-magnetic metal layer, which absorbs a pump laser pulse. Demagnetization by electronic heating is investigated on samples with different thicknesses of the absorber layer on nickel. This allows us to separate the contribution of thermalized hot electrons compared to non-thermal electrons. An analytical model describes the demagnetization amplitude as a function of the absorber thickness. The observed change of demagnetization time can be reproduced by diffusive heat transport through the absorber layer.

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.

Ultrafast electronic relaxation in superheated bismuth

NASA Astrophysics Data System (ADS)

Gamaly, E. G.; Rode, A. V.

2013-01-01

Interaction of moving electrons with vibrating ions in the lattice forms the basis for many physical properties from electrical resistivity and electronic heat capacity to superconductivity. In ultrafast laser interaction with matter the electrons are heated much faster than the electron-ion energy equilibration, leading to a two-temperature state with electron temperature far above that of the lattice. The rate of temperature equilibration is governed by the strength of electron-phonon energy coupling, which is conventionally described by a coupling constant, neglecting the dependence on the electron and lattice temperature. The application of this constant to the observations of fast relaxation rate led to a controversial notion of ‘ultra-fast non-thermal melting’ under extreme electronic excitation. Here we provide theoretical grounds for a strong dependence of the electron-phonon relaxation time on the lattice temperature. We show, by taking proper account of temperature dependence, that the heating and restructuring of the lattice occurs much faster than were predicted on the assumption of a constant, temperature independent energy coupling. We applied the temperature-dependent momentum and energy transfer time to experiments on fs-laser excited bismuth to demonstrate that all the observed ultra-fast transformations of the transient state of bismuth are purely thermal in nature. The developed theory, when applied to ultrafast experiments on bismuth, provides interpretation of the whole variety of transient phase relaxation without the non-thermal melting conjecture.

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.

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.

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.

Probing ultrafast spin dynamics through a magnon resonance in the antiferromagnetic multiferroic HoMnO 3

DOE PAGES

Bowlan, P.; Trugman, S. A.; Bowlan, J.; ...

2016-09-26

Here, we demonstrate an approach for directly tracking antiferromagnetic (AFM) spin dynamics by measuring ultrafast changes in a magnon resonance. We also test this idea on the multiferroic HoMnO 3 by optically photoexciting electrons, after which changes in the spin order are probed with a THz pulse tuned to a magnon resonance. This reveals a photoinduced change in the magnon line shape that builds up over 5–12 picoseconds, which we show to be the spin-lattice thermalization time, indicating that electrons heat the spins via phonons. We compare our results to previous studies of spin-lattice thermalization in ferromagnetic manganites, giving insightmore » into fundamental differences between the two systems. Finally, our work sheds light on the microscopic mechanism governing spin-phonon interactions in AFMs and demonstrates a powerful approach for directly monitoring ultrafast spin dynamics.« less

Precision machining of pig intestine using ultrafast laser pulses

NASA Astrophysics Data System (ADS)

Beck, Rainer J.; Góra, Wojciech S.; Carter, Richard M.; Gunadi, Sonny; Jayne, David; Hand, Duncan P.; Shephard, Jonathan D.

2015-07-01

Endoluminal surgery for the treatment of early stage colorectal cancer is typically based on electrocautery tools which imply restrictions on precision and the risk of harm through collateral thermal damage to the healthy tissue. As a potential alternative to mitigate these drawbacks we present laser machining of pig intestine by means of picosecond laser pulses. The high intensities of an ultrafast laser enable nonlinear absorption processes and a predominantly nonthermal ablation regime. Laser ablation results of square cavities with comparable thickness to early stage colorectal cancers are presented for a wavelength of 1030 nm using an industrial picosecond laser. The corresponding histology sections exhibit only minimal collateral damage to the surrounding tissue. The depth of the ablation can be controlled precisely by means of the pulse energy. Overall, the application of ultrafast lasers to ablate pig intestine enables significantly improved precision and reduced thermal damage to the surrounding tissue compared to conventional techniques.

Probing ultrafast spin dynamics through a magnon resonance in the antiferromagnetic multiferroic HoMnO 3

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

Bowlan, P.; Trugman, S. A.; Bowlan, J.

Here, we demonstrate an approach for directly tracking antiferromagnetic (AFM) spin dynamics by measuring ultrafast changes in a magnon resonance. We also test this idea on the multiferroic HoMnO 3 by optically photoexciting electrons, after which changes in the spin order are probed with a THz pulse tuned to a magnon resonance. This reveals a photoinduced change in the magnon line shape that builds up over 5–12 picoseconds, which we show to be the spin-lattice thermalization time, indicating that electrons heat the spins via phonons. We compare our results to previous studies of spin-lattice thermalization in ferromagnetic manganites, giving insightmore » into fundamental differences between the two systems. Finally, our work sheds light on the microscopic mechanism governing spin-phonon interactions in AFMs and demonstrates a powerful approach for directly monitoring ultrafast spin dynamics.« less

Ultrafast time-resolved electron diffraction revealing the nonthermal dynamics of near-UV photoexcitation-induced amorphization in Ge2Sb2Te5.

PubMed

Hada, Masaki; Oba, Wataru; Kuwahara, Masashi; Katayama, Ikufumi; Saiki, Toshiharu; Takeda, Jun; Nakamura, Kazutaka G

2015-08-28

Because of their robust switching capability, chalcogenide glass materials have been used for a wide range of applications, including optical storages devices. These phase transitions are achieved by laser irradiation via thermal processes. Recent studies have suggested the potential of nonthermal phase transitions in the chalcogenide glass material Ge2Sb2Te5 triggered by ultrashort optical pulses; however, a detailed understanding of the amorphization and damage mechanisms governed by nonthermal processes is still lacking. Here we performed ultrafast time-resolved electron diffraction and single-shot optical pump-probe measurements followed by femtosecond near-ultraviolet pulse irradiation to study the structural dynamics of polycrystalline Ge2Sb2Te5. The experimental results present a nonthermal crystal-to-amorphous phase transition of Ge2Sb2Te5 initiated by the displacements of Ge atoms. Above the fluence threshold, we found that the permanent amorphization caused by multi-displacement effects is accompanied by a partial hexagonal crystallization.

Ultrafast time-resolved electron diffraction revealing the nonthermal dynamics of near-UV photoexcitation-induced amorphization in Ge2Sb2Te5

PubMed Central

Hada, Masaki; Oba, Wataru; Kuwahara, Masashi; Katayama, Ikufumi; Saiki, Toshiharu; Takeda, Jun; Nakamura, Kazutaka G.

2015-01-01

Because of their robust switching capability, chalcogenide glass materials have been used for a wide range of applications, including optical storages devices. These phase transitions are achieved by laser irradiation via thermal processes. Recent studies have suggested the potential of nonthermal phase transitions in the chalcogenide glass material Ge2Sb2Te5 triggered by ultrashort optical pulses; however, a detailed understanding of the amorphization and damage mechanisms governed by nonthermal processes is still lacking. Here we performed ultrafast time-resolved electron diffraction and single-shot optical pump-probe measurements followed by femtosecond near-ultraviolet pulse irradiation to study the structural dynamics of polycrystalline Ge2Sb2Te5. The experimental results present a nonthermal crystal-to-amorphous phase transition of Ge2Sb2Te5 initiated by the displacements of Ge atoms. Above the fluence threshold, we found that the permanent amorphization caused by multi-displacement effects is accompanied by a partial hexagonal crystallization. PMID:26314613

Ultrafast Chemistry under Nonequilibrium Conditions and the Shock to Deflagration Transition at the Nanoscale

DOE PAGES

Wood, Mitchell A.; Cherukara, Mathew J.; Kober, Edward M.; ...

2015-06-13

We use molecular dynamics simulations to describe the chemical reactions following shock-induced collapse of cylindrical pores in the high-energy density material RDX. For shocks with particle velocities of 2 km/s we find that the collapse of a 40 nm diameter pore leads to a deflagration wave. Molecular collisions during the collapse lead to ultrafast, multistep chemical reactions that occur under nonequilibrium conditions. WE found that exothermic products formed during these first few picoseconds prevent the nanoscale hotspot from quenching. Within 30 ps, a local deflagration wave develops. It propagates at 0.25 km/s and consists of an ultrathin reaction zone ofmore » only ~5 nm, thus involving large temperature and composition gradients. Contrary to the assumptions in current models, a static thermal hotspot matching the dynamical one in size and thermodynamic conditions fails to produce a deflagration wave indicating the importance of nonequilibrium loading in the criticality of nanoscale hot spots. These results provide insight into the initiation of reactive decomposition.« 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.

Observation of ultrafast temporal evolution of symmetry in short-pulsed laser induced transient states of matter (Conference Presentation)

NASA Astrophysics Data System (ADS)

Garnett, Joy; Krzyzanowska, Halina; Baydin, Andrey; Tolk, Norman H.

2017-02-01

In condensed matter physics, ultrafast photoexcitation has been shown to result in modification of macroscopic material properties, sometimes involving phase changes, on a subpicosecond time scale. In semiconductors, irreversible non-thermal solid-to-liquid structural transitions have been demonstrated at high laser fluences. In the pump-probe experiments reported here, we observe a striking continuously varying low-fluence pump-induced time-dependent structural symmetry modification in intrinsic gallium arsenide (GaAs) using a probe that produces femtosecond polarization-resolved second harmonic generation (f-PRSHG) data. SHG spectroscopy is particularly suited to monitor symmetry changes since its magnitude is governed by the nonlinear optical susceptibility tensor whose elements are determined by the underlying material symmetry. Conceptually, these experiments seek to provide insight into the details of the time evolution of symmetry arising from laser induced transient states of matter in GaAs. Overall, the basic explanation of these experimental observations is that as a result of the photoinduced electronic excitation, many electrons, including bond electrons are excited to higher states. This results in subpicosecond changes in the local anharmonic potential and produces a changing nonlinear polarization response thus accounting for the nonthermal time dependent symmetry changes. Clearly, our approach may be easily extended to many different crystalline materials with different levels of defects, dopants and stresses to fully characterize the time dependent behavior of laser induced transient states in material systems.

The indispensable role of the transversal spin fluctuations mechanism in laser-induced demagnetization of Co/Pt multilayers with nanoscale magnetic domains.

PubMed

Zhang, Wei; He, Wei; Peng, Li-Cong; Zhang, Ying; Cai, Jian-Wang; Evans, Richard F L; Zhang, Xiang-Qun; Cheng, Zhao-Hua

2018-07-06

The switching of magnetic domains induced by an ultrashort laser pulse has been demonstrated in nanostructured ferromagnetic films. This leads to the dawn of a new era in breaking the ultimate physical limit for the speed of magnetic switching and manipulation, which is relevant to current and future information storage. However, our understanding of the interactions between light and spins in magnetic heterostructures with nanoscale domain structures is still lacking. Here, both time-resolved magneto-optical Kerr effect experiments and atomistic simulations are carried out to investigate the dominant mechanism of laser-induced ultrafast demagnetization in [Co/Pt] 20 multilayers with nanoscale magnetic domains. It is found that the ultrafast demagnetization time remains constant with various magnetic configurations, indicating that the domain structures play a minor role in laser-induced ultrafast demagnetization. In addition, both in experiment and atomistic simulations, we find a dependence of ultrafast demagnetization time τ M on the laser fluence, which is in contrast to the observations of spin transport within magnetic domains. The remarkable agreement between experiment and atomistic simulations indicates that the local dissipation of spin angular momentum is the dominant demagnetization mechanism in this system. More interestingly, we made a comparison between the atomistic spin dynamic simulation and the longitudinal spin flip model, highlighting that the transversal spin fluctuations mechanism is responsible for the ultrafast demagnetization in the case of inhomogeneous magnetic structures. This is a significant advance in clarifying the microscopic mechanism underlying the process of ultrafast demagnetization in inhomogeneous magnetic structures.

Vanishing Thermal Conductance of Carbon Nanotube upon Encapsulation by Zigzag Sulfur Chain.

PubMed

Koley, Sayantanu; Sen, Sabyasachi; Chakrabarti, Swapan

2018-06-07

We report an unprecedented enhancement of thermoelectric properties of a single-walled carbon nanotube upon encapsulation of a zigzag sulfur chain inside the nanocore. Our calculations on a 70 Å long [5, 5] carbon nanotube reveal that the encapsulation of zigzag sulfur chain will lead to a 10 7 % increase in the thermoelectric figure of merit and concomitant quenching of thermal conductance by 90%. We have noticed that finite transmission gradient at the Fermi level combined with destructive quantum interference at the sulfur sites and structural conformation-dependent scattering-induced damping of phonon transmission are attributed to the dramatic improvement of thermoelectric behavior of this material. This finding indeed will help circumvent the long-standing problem in the fabrication of carbon-nanotube-based ultrafast device.

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.

Vibrational energy on surfaces: Ultrafast flash-thermal conductance of molecular monolayers

NASA Astrophysics Data System (ADS)

Dlott, Dana

2008-03-01

Vibrational energy flow through molecules remains a perennial problem in chemical physics. Usually vibrational energy dynamics are viewed through the lens of time-dependent level populations. This is natural because lasers naturally pump and probe vibrational transitions, but it is also useful to think of vibrational energy as being conducted from one location in a molecule to another. We have developed a new technique where energy is driven into a specific part of molecules adsorbed on a metal surface, and ultrafast nonlinear coherent vibrational spectroscopy is used to watch the energy arrive at another part. This technique is the analog of a flash thermal conductance apparatus, except it probes energy flow with angstrom spatial and femtosecond temporal resolution. Specific examples to be presented include energy flow along alkane chains, and energy flow into substituted benzenes. Ref: Z. Wang, J. A. Carter, A. Lagutchev, Y. K. Koh, N.-H. Seong, D. G. Cahill, and D. D. Dlott, Ultrafast flash thermal conductance of molecular chains, Science 317, 787-790 (2007). This material is based upon work supported by the National Science Foundation under award DMR 0504038 and the Air Force Office of Scientific Research under award FA9550-06-1-0235.

Thermal or nonthermal? That is the question for ultrafast spin switching in GdFeCo.

PubMed

Zhang, G P; George, Thomas F

2013-09-11

GdFeCo is among the most interesting magnets for producing laser-induced femtosecond magnetism, where light can switch its spin moment from one direction to another. This paper aims to set a criterion for the thermal/nonthermal mechanism: we propose to use the Fermi-Dirac distribution function as a reliable criterion. A precise value for the thermalization time is needed, and through a two-level model, we show that since there is no direct connection between the laser helicity and the definition of thermal/nonthermal processes, the helicity is a poor criterion for differentiating a thermal from a nonthermal process. In addition, we propose a four-site model system (Gd2Fe2) for investigating the transient ferromagnetic ordering between Gd and Fe ions. We find that states of two different kinds can allow such an ordering. One state is a pure ferromagnetic state with ferromagnetic ordering among all the ions, and the other is the short-ranged ferromagnetic ordering of a pair of Gd and Fe ions.

Protonation-induced ultrafast torsional dynamics in 9-anthrylbenzimidazole: a pH activated molecular rotor.

PubMed

Nandi, Amitabha; Kushwaha, Archana; Das, Dipanwita; Ghosh, Rajib

2018-03-07

We report the photophysical properties and excited state dynamics of 9-anthrylbenzimidazole (ANBI) which exhibits protonation-induced molecular rotor properties. In contrast to the highly emissive behavior of neutral ANBI, protonation of the benzimidazole group of ANBI induces efficient nonradiative deactivation by ultrafast torsional motion around the bond connecting the anthracene and benzimidazole units, as revealed by ultrafast transient absorption and fluorescence spectroscopy. Contrary to viscosity-independent fluorescence of neutral dyes, protonated ANBI is shown to display linear variation of emission yield and lifetime with solvent viscosity. The protonation-induced molecular rotor properties in the studied system are shown to be driven by enhanced charge transfer and are corroborated by quantum chemical calculations. Potential application as a microviscosity sensor of acidic regions in a heterogeneous environment by these proton-activated molecular rotor properties of ANBI is discussed.

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 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. Electronic supplementary information (ESI) available: Electron scattering patterns from TEM characterizations of MX2 nanosheets; CA Z-scan results of graphene dispersions in the ps region. See DOI: 10.1039/c4nr02634a

Ultrafast Spreading Effect Induced Rapid Cell Trapping into Porous Scaffold with Superhydrophilic Surface.

PubMed

Wang, Chenmiao; Qiao, Chunyan; Song, Wenlong; Sun, Hongchen

2015-08-19

In this contribution, superhydrophilic chitosan-based scaffolds with ultrafast spreading property were fabricated and used to improve the trapped efficiency of cells. The ultrafast spreading property allowed cells to be trapped into the internal 3D porous structures of the prepared scaffolds more quickly and effectively. Cell adhesion, growth, and proliferation were also improved, which could be attributed to the combination of UV irradiation and ultrafast spreading property. The construction of ultrafast spreading property on the scaffold surface will offer a novel way to design more effective scaffold in tissue engineering that could largely shorten the therapeutic time for patients.

Strong-Field Control of Laser Filamentation Mechanisms

NASA Astrophysics Data System (ADS)

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

2008-05-01

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

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 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.

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 controlled magnetic switching. Our results present a fundamentally new switching mechanism electrically, without requirement for any spin polarized current or spin transfer/orbit torques. Our discovery that ultrafast magnetization switching can be achieved with electrical pulses will launch a new frontier of spintronics science and herald a new generation of spintronic devices that operate at high speed with low energy consumption. At last, to push ultrafast spintronics to practical use, ultrafast switching of a ferromagnetic film is desired. By exploiting the exchange interaction between GdFeCo and ferromagnetic Co/Pt layer, we achieved ultrafast (sub 10ps) switching of ferromagnetic film with a single laser pulse. This result will open up the possibility to control ferromagnetic materials at ultrafast time scale, critical for practical applications.

Measuring thermal conductivity of thin films and coatings with the ultra-fast transient hot-strip technique

NASA Astrophysics Data System (ADS)

Belkerk, B. E.; Soussou, M. A.; Carette, M.; Djouadi, M. A.; Scudeller, Y.

2012-07-01

This paper reports the ultra-fast transient hot-strip (THS) technique for determining the thermal conductivity of thin films and coatings of materials on substrates. The film thicknesses can vary between 10 nm and more than 10 µm. Precise measurement of thermal conductivity was performed with an experimental device generating ultra-short electrical pulses, and subsequent temperature increases were electrically measured on nanosecond and microsecond time scales. The electrical pulses were applied within metallized micro-strips patterned on the sample films and the temperature increases were analysed within time periods selected in the window [100 ns-10 µs]. The thermal conductivity of the films was extracted from the time-dependent thermal impedance of the samples derived from a three-dimensional heat diffusion model. The technique is described and its performance demonstrated on different materials covering a large thermal conductivity range. Experiments were carried out on bulk Si and thin films of amorphous SiO2 and crystallized aluminum nitride (AlN). The present approach can assess film thermal resistances as low as 10-8 K m2 W-1 with a precision of about 10%. This has never been attained before with the THS technique.

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.

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.

Development of functional materials by using ultrafast laser pulses

NASA Astrophysics Data System (ADS)

Shimotsuma, Y.; Sakakura, M.; Miura, K.

2018-01-01

The polarization-dependent periodic nanostructures inside various materials are successfully induced by ultrafast laser pulses. The periodic nanostructures in various materials can be empirically classified into the following three types: (1) structural deficiency, (2) expanded structure, (3) partial phase separation. Such periodic nanostructures exhibited not only optical anisotropy but also intriguing electric, thermal, and magnetic properties. The formation mechanisms of the periodic nanostructure was interpreted in terms of the interaction between incident light field and the generated electron plasma. Furthermore, the fact that the periodic nanostructures in semiconductors could be formed empirically only if it is indirect bandgap semiconductor materials indicates the stress-dependence of bandgap structure and/or the recombination of the excited electrons are also involved to the nanostructure formation. More recently we have also confirmed that the periodic nanostructures in glass are related to whether a large amount of non-bridged oxygen is present. In the presentation, we demonstrate new possibilities for functionalization of common materials ranging from an eternal 5D optical storage, a polarization imaging, to a thermoelectric conversion, based on the indicated phenomena.

Ultrafast evolution and transient phases of a prototype out-of-equilibrium Mott–Hubbard material

DOE PAGES

Lantz, G.; Mansart, B.; Grieger, D.; ...

2017-01-09

Photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behavior, including non-thermal phases and photoinduced phase transitions. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states of matter inaccessible by quasi-adiabatic pathways. We present a study of the ultrafast non-equilibrium evolution of the prototype Mott-Hubbard material V 2O 3, which presents a transient non-thermal phase developing immediately after photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configurationmore » is triggered by the excitation of electrons into the bonding a 1g orbital, and is then stabilized by a lattice distortion characterized by a marked hardening of the A 1g coherent phonon. Furthermore, this configuration is in stark contrast with the thermally accessible ones - the A 1g phonon frequency actually softens when heating the material. Our results show the importance of selective electron-lattice interplay for the ultrafast control of material parameters, and are of particular relevance for the optical manipulation of strongly correlated systems, whose electronic and structural properties are often strongly intertwinned.« less

Ultrafast evolution and transient phases of a prototype out-of-equilibrium Mott–Hubbard material

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

Lantz, G.; Mansart, B.; Grieger, D.

Photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behavior, including non-thermal phases and photoinduced phase transitions. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states of matter inaccessible by quasi-adiabatic pathways. We present a study of the ultrafast non-equilibrium evolution of the prototype Mott-Hubbard material V 2O 3, which presents a transient non-thermal phase developing immediately after photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configurationmore » is triggered by the excitation of electrons into the bonding a 1g orbital, and is then stabilized by a lattice distortion characterized by a marked hardening of the A 1g coherent phonon. Furthermore, this configuration is in stark contrast with the thermally accessible ones - the A 1g phonon frequency actually softens when heating the material. Our results show the importance of selective electron-lattice interplay for the ultrafast control of material parameters, and are of particular relevance for the optical manipulation of strongly correlated systems, whose electronic and structural properties are often strongly intertwinned.« less

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

Kay, Jeffrey J.; Park, Samuel; Kohl, Ian Thomas

In this work, shock-induced reactions in high explosives and their chemical mechanisms were investigated using state-of-the-art experimental and theoretical techniques. Experimentally, ultrafast shock interrogation (USI, an ultrafast interferometry technique) and ultrafast absorption spectroscopy were used to interrogate shock compression and initiation of reaction on the picosecond timescale. The experiments yielded important new data that appear to indicate reaction of high explosives on the timescale of tens of picoseconds in response to shock compression, potentially setting new upper limits on the timescale of reaction. Theoretically, chemical mechanisms of shock-induced reactions were investigated using density functional theory. The calculations generated important insightsmore » regarding the ability of several hypothesized mechanisms to account for shock-induced reactions in explosive materials. The results of this work constitute significant advances in our understanding of the fundamental chemical reaction mechanisms that control explosive sensitivity and initiation of detonation.« less

Sensing Atomic Motion from the Zero Point to Room Temperature with Ultrafast Atom Interferometry.

PubMed

Johnson, K G; Neyenhuis, B; Mizrahi, J; Wong-Campos, J D; Monroe, C

2015-11-20

We sense the motion of a trapped atomic ion using a sequence of state-dependent ultrafast momentum kicks. We use this atom interferometer to characterize a nearly pure quantum state with n=1 phonon and accurately measure thermal states ranging from near the zero-point energy to n[over ¯]~10^{4}, with the possibility of extending at least 100 times higher in energy. The complete energy range of this method spans from the ground state to far outside of the Lamb-Dicke regime, where atomic motion is greater than the optical wavelength. Apart from thermometry, these interferometric techniques are useful for characterizing ultrafast entangling gates between multiple trapped ions.

Photoinduced surface plasmon switching at VO2/Au interface.

PubMed

Kumar, Nardeep; Rúa, Armando; Aldama, Jennifer; Echeverría, Karla; Fernández, Félix E; Lysenko, Sergiy

2018-05-28

Angle-resolved reflection, light scattering and ultrafast pump-probe spectroscopy combined with a surface plasmon-polariton (SPP) resonance technique in attenuated total reflection geometry was used to investigate the light-induced plasmonic switching in a photorefractive VO 2 /Au hybrid structure. Measurements of SPP scattering and reflection shows that the optically-induced formation of metallic state in a vanadium dioxide layer deposited on a gold film significantly alters the electromagnetic field enhancement and SPP propagation length at the VO 2 /Au interface. The ultrafast optical manipulation of SPP resonance is shown on a picosecond timescale. Obtained results demonstrate high potential of photorefractive vanadium oxides as efficient plasmonic modulating materials for ultrafast optoelectronic devices.

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.

Electronic and nuclear contributions to time-resolved optical and X-ray absorption spectra of hematite and insights into photoelectrochemical performance

DOE PAGES

Hayes, Dugan; Hadt, Ryan G.; Emery, Jonathan D.; ...

2016-11-02

Ultrafast time-resolved studies of photocatalytic thin films can provide a wealth of information crucial for understanding and thereby improving the performance of these materials by directly probing electronic structure, reaction intermediates, and charge carrier dynamics. The interpretation of transient spectra, however, can be complicated by thermally induced structural distortions, which appear within the first few picoseconds following excitation due to carrier–phonon scattering. Here we present a comparison of ex situ steady-state thermal difference spectra and transient absorption spectra spanning from NIR to hard X-ray energies of hematite thin films grown by atomic layer deposition. We find that beyond the firstmore » 100 picoseconds, the transient spectra measured for all excitation wavelengths and probe energies are almost entirely due to thermal effects as the lattice expands in response to the ultrafast temperature jump and then cools to room temperature on the microsecond timescale. At earlier times, a broad excited state absorption band that is assigned to free carriers appears at 675 nm, and the lifetime and shape of this feature also appear to be mostly independent of excitation wavelength. The combined spectroscopic data, which are modeled with density functional theory and full multiple scattering calculations, support an assignment of the optical absorption spectrum of hematite that involves two LMCT bands that nearly span the visible spectrum. Lastly, our results also suggest a framework for shifting the ligand-to-metal charge transfer absorption bands of ferric oxide films from the near-UV further into the visible part of the solar spectrum to improve solar conversion efficiency.« less

Ultrafast pulsed laser utilizing broad bandwidth laser glass

DOEpatents

Payne, Stephen A.; Hayden, Joseph S.

1997-01-01

An ultrafast laser uses a Nd-doped phosphate laser glass characterized by a particularly broad emission bandwidth to generate the shortest possible output pulses. The laser glass is composed primarily of P.sub.2 O.sub.5, Al.sub.2 O.sub.3 and MgO, and possesses physical and thermal properties that are compatible with standard melting and manufacturing methods. The broad bandwidth laser glass can be used in modelocked oscillators as well as in amplifier modules.

Nanoscale electron manipulation in metals with intense THz electric fields

NASA Astrophysics Data System (ADS)

Takeda, Jun; Yoshioka, Katsumasa; Minami, Yasuo; Katayama, Ikufumi

2018-03-01

Improved control over the electromagnetic properties of metals on a nanoscale is crucial for the development of next-generation nanoelectronics and plasmonic devices. Harnessing the terahertz (THz)-electric-field-induced nonlinearity for the motion of electrons is a promising method of manipulating the local electromagnetic properties of metals, while avoiding undesirable thermal effects and electronic transitions. In this review, we demonstrate the manipulation of electron delocalization in ultrathin gold (Au) films with nanostructures, by intense THz electric-field transients. On increasing the electric-field strength of the THz pulses, the transmittance in the THz-frequency region abruptly decreases around the percolation threshold. The observed THz-electric-field-induced nonlinearity is analysed, based on the Drude-Smith model. The results suggest that ultrafast electron delocalization occurs by electron tunnelling across the narrow insulating bridge between the Au nanostructures, without material breakdown. In order to quantitatively discuss the tunnelling process, we perform scanning tunnelling microscopy with carrier-envelope phase (CEP)-controlled single-cycle THz electric fields. By applying CEP-controlled THz electric fields to the 1 nm nanogap between a metal nanotip and graphite sample, many electrons could be coherently driven through the quantum tunnelling process, either from the nanotip to the sample or vice versa. The presented concept, namely, electron tunnelling mediated by CEP-controlled single-cycle THz electric fields, can facilitate the development of nanoscale electron manipulation, applicable to next-generation ultrafast nanoelectronics and plasmonic devices.

Spatial Temperature Mapping within Polymer Nanocomposites Undergoing Ultrafast Photothermal Heating via Gold Nanorods

PubMed Central

Maity, Somsubhra; Wu, Wei-Chen; Xu, Chao; Tracy, Joseph B.; Gundogdu, Kenan; Bochinski, Jason R.; Clarke, Laura I.

2015-01-01

Heat emanates from gold nanorods (GNRs) under ultrafast optical excitation of the localized surface plasmon resonance. The steady state nanoscale temperature distribution formed within a polymer matrix embedded with GNRs undergoing pulsed femtosecond photothermal heating is determined experimentally using two independent ensemble optical techniques. Physical rotation of the nanorods reveals the average local temperature of the polymer melt in the immediate spatial volume surrounding them while fluorescence of homogeneously-distributed perylene molecules monitors temperature over sample regions at larger distances from the GNRs. Polarization-sensitive fluorescence measurements of the perylene probes provide an estimate of the average size of the quasi-molten region surrounding each nanorod (that is, the boundary between softened polymer and solid material as the temperature decreases radially away from each particle) and distinguishes the steady state temperature in the solid and melt regions. Combining these separate methods enables nanoscale spatial mapping of the average steady state temperature distribution caused by ultrafast excitation of the GNRs. These observations definitively demonstrate the presence of a steady-state temperature gradient and indicate that localized heating via the photothermal effect within materials enables nanoscale thermal manipulations without significantly altering the bulk sample temperature in these systems. These quantitative results are further verified by reorienting nanorods within a solid polymer nanofiber without inducing any morphological changes to the highly temperature-sensitive nanofiber surface. Temperature differences of 70 – 90 °C were observed over a distances of ~100 nm. PMID:25379775

Anomalous ultrafast dynamics of hot plasmonic electrons in nanostructures with hot spots

DOE PAGES

Harutyunyan, Hayk; Martinson, Alex B. F.; Rosenmann, Daniel; ...

2015-08-03

The interaction of light and matter in metallic nanosystems is mediated by the collective oscillation of surface electrons, called plasmons. After excitation, plasmons are absorbed by the metal electrons through inter- and intraband transitions, creating a highly non-thermal distribution of electrons. The electron population then decays through electron-electron interactions, creating a hot electron distribution within a few hundred femtoseconds, followed by a further relaxation via electron-phonon scattering on the timescale of a few pico-seconds. In the spectral domain, hot plasmonic electrons induce changes to the plasmonic resonance of the nanostructure by modifying the dielectric constant of the metal. Here, wemore » report on the observation of anomalously strong changes to the ultrafast temporal and spectral responses of these excited hot plasmonic electrons in hybrid metal/oxide nanostructures as a result of varying the geometry and composition of the nanostructure and the excitation wavelength. In particular, we show a large ultrafast, pulsewidth-limited contribution to the excited electron decay signal in hybrid nanostructures containing hot spots. The intensity of this contribution correlates with the efficiency of the generation of highly excited surface electrons. Using theoretical models, we attribute this effect to the generation of hot plasmonic electrons from hot spots. Finally, we then develop general principles to enhance the generation of energetic electrons through specifically designed plasmonic nanostructures that could be used in applications where hot electron generation is beneficial, such as in solar photocatalysis, photodetectors and nonlinear devices.« less

Anomalous ultrafast dynamics of hot plasmonic electrons in nanostructures with hot spots.

PubMed

Harutyunyan, Hayk; Martinson, Alex B F; Rosenmann, Daniel; Khorashad, Larousse Khosravi; Besteiro, Lucas V; Govorov, Alexander O; Wiederrecht, Gary P

2015-09-01

The interaction of light and matter in metallic nanosystems is mediated by the collective oscillation of surface electrons, called plasmons. After excitation, plasmons are absorbed by the metal electrons through inter- and intraband transitions, creating a highly non-thermal distribution of electrons. The electron population then decays through electron-electron interactions, creating a hot electron distribution within a few hundred femtoseconds, followed by a further relaxation via electron-phonon scattering on the timescale of a few picoseconds. In the spectral domain, hot plasmonic electrons induce changes to the plasmonic resonance of the nanostructure by modifying the dielectric constant of the metal. Here, we report on the observation of anomalously strong changes to the ultrafast temporal and spectral responses of these excited hot plasmonic electrons in hybrid metal/oxide nanostructures as a result of varying the geometry and composition of the nanostructure and the excitation wavelength. In particular, we show a large ultrafast, pulsewidth-limited contribution to the excited electron decay signal in hybrid nanostructures containing hot spots. The intensity of this contribution correlates with the efficiency of the generation of highly excited surface electrons. Using theoretical models, we attribute this effect to the generation of hot plasmonic electrons from hot spots. We then develop general principles to enhance the generation of energetic electrons through specifically designed plasmonic nanostructures that could be used in applications where hot electron generation is beneficial, such as in solar photocatalysis, photodetectors and nonlinear devices.

Ultrafast dynamics induced by the interaction of molecules with electromagnetic fields: Several quantum, semiclassical, and classical approaches.

PubMed

Antipov, Sergey V; Bhattacharyya, Swarnendu; El Hage, Krystel; Xu, Zhen-Hao; Meuwly, Markus; Rothlisberger, Ursula; Vaníček, Jiří

2017-11-01

Several strategies for simulating the ultrafast dynamics of molecules induced by interactions with electromagnetic fields are presented. After a brief overview of the theory of molecule-field interaction, we present several representative examples of quantum, semiclassical, and classical approaches to describe the ultrafast molecular dynamics, including the multiconfiguration time-dependent Hartree method, Bohmian dynamics, local control theory, semiclassical thawed Gaussian approximation, phase averaging, dephasing representation, molecular mechanics with proton transfer, and multipolar force fields. In addition to the general overview, some focus is given to the description of nuclear quantum effects and to the direct dynamics, in which the ab initio energies and forces acting on the nuclei are evaluated on the fly. Several practical applications, performed within the framework of the Swiss National Center of Competence in Research "Molecular Ultrafast Science and Technology," are presented: These include Bohmian dynamics description of the collision of H with H 2 , local control theory applied to the photoinduced ultrafast intramolecular proton transfer, semiclassical evaluation of vibrationally resolved electronic absorption, emission, photoelectron, and time-resolved stimulated emission spectra, infrared spectroscopy of H-bonding systems, and multipolar force fields applications in the condensed phase.

Ultrafast dynamics induced by the interaction of molecules with electromagnetic fields: Several quantum, semiclassical, and classical approaches

PubMed Central

Antipov, Sergey V.; Bhattacharyya, Swarnendu; El Hage, Krystel; Xu, Zhen-Hao; Meuwly, Markus; Rothlisberger, Ursula; Vaníček, Jiří

2018-01-01

Several strategies for simulating the ultrafast dynamics of molecules induced by interactions with electromagnetic fields are presented. After a brief overview of the theory of molecule-field interaction, we present several representative examples of quantum, semiclassical, and classical approaches to describe the ultrafast molecular dynamics, including the multiconfiguration time-dependent Hartree method, Bohmian dynamics, local control theory, semiclassical thawed Gaussian approximation, phase averaging, dephasing representation, molecular mechanics with proton transfer, and multipolar force fields. In addition to the general overview, some focus is given to the description of nuclear quantum effects and to the direct dynamics, in which the ab initio energies and forces acting on the nuclei are evaluated on the fly. Several practical applications, performed within the framework of the Swiss National Center of Competence in Research “Molecular Ultrafast Science and Technology,” are presented: These include Bohmian dynamics description of the collision of H with H2, local control theory applied to the photoinduced ultrafast intramolecular proton transfer, semiclassical evaluation of vibrationally resolved electronic absorption, emission, photoelectron, and time-resolved stimulated emission spectra, infrared spectroscopy of H-bonding systems, and multipolar force fields applications in the condensed phase. PMID:29376107

Glass-Like Through-Plane Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La 0.5Sr 0.5CoO 3– δ [Glass-Like Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La 0.5Sr 0.5CoO 3– δ

DOE PAGES

Wu, Xuewang; Walter, Jeff; Feng, Tianli; ...

2017-11-02

Here, ultrafast time-domain thermoreflectance (TDTR) is utilized to extract the through-plane thermal conductivity (Λ LSCO) of epitaxial La 0.5Sr 0.5CoO 3–δ (LSCO) of varying thickness (<20 nm) on LaAlO 3 and SrTiO 3 substrates. These LSCO films possess ordered oxygen vacancies as the primary means of lattice mismatch accommodation with the substrate, which induces compressive/tensile strain and thus controls the orientation of the oxygen vacancy ordering (OVO). TDTR results demonstrate that the room-temperature Λ LSCO of LSCO on both substrates (1.7 W m –1 K –1) are nearly a factor of four lower than that of bulk single-crystal LSCO (6.2more » W m –1 K –1). Remarkably, this approaches the lower limit of amorphous oxides (e.g., 1.3 W m –1 K –1 for glass), with no dependence on the OVO orientation. Through theoretical simulations, origins of the glass-like thermal conductivity of LSCO are revealed as a combined effect resulting from oxygen vacancies (the dominant factor), Sr substitution, size effects, and the weak electron/phonon coupling within the LSCO film. The absence of OVO dependence in the measured Λ LSCO is rationalized by two main effects: (1) the nearly isotropic phononic thermal conductivity resulting from the imperfect OVO planes when δ is small; (2) the missing electronic contribution to Λ LSCO along the through-plane direction for these ultrathin LSCO films on insulating substrates.« less

Glass-Like Through-Plane Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La 0.5Sr 0.5CoO 3– δ [Glass-Like Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La 0.5Sr 0.5CoO 3– δ

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

Wu, Xuewang; Walter, Jeff; Feng, Tianli

Here, ultrafast time-domain thermoreflectance (TDTR) is utilized to extract the through-plane thermal conductivity (Λ LSCO) of epitaxial La 0.5Sr 0.5CoO 3–δ (LSCO) of varying thickness (<20 nm) on LaAlO 3 and SrTiO 3 substrates. These LSCO films possess ordered oxygen vacancies as the primary means of lattice mismatch accommodation with the substrate, which induces compressive/tensile strain and thus controls the orientation of the oxygen vacancy ordering (OVO). TDTR results demonstrate that the room-temperature Λ LSCO of LSCO on both substrates (1.7 W m –1 K –1) are nearly a factor of four lower than that of bulk single-crystal LSCO (6.2more » W m –1 K –1). Remarkably, this approaches the lower limit of amorphous oxides (e.g., 1.3 W m –1 K –1 for glass), with no dependence on the OVO orientation. Through theoretical simulations, origins of the glass-like thermal conductivity of LSCO are revealed as a combined effect resulting from oxygen vacancies (the dominant factor), Sr substitution, size effects, and the weak electron/phonon coupling within the LSCO film. The absence of OVO dependence in the measured Λ LSCO is rationalized by two main effects: (1) the nearly isotropic phononic thermal conductivity resulting from the imperfect OVO planes when δ is small; (2) the missing electronic contribution to Λ LSCO along the through-plane direction for these ultrathin LSCO films on insulating substrates.« less

Ultrafast pulsed laser utilizing broad bandwidth laser glass

DOEpatents

Payne, S.A.; Hayden, J.S.

1997-09-02

An ultrafast laser uses a Nd-doped phosphate laser glass characterized by a particularly broad emission bandwidth to generate the shortest possible output pulses. The laser glass is composed primarily of P{sub 2}O{sub 5}, Al{sub 2}O{sub 3} and MgO, and possesses physical and thermal properties that are compatible with standard melting and manufacturing methods. The broad bandwidth laser glass can be used in modelocked oscillators as well as in amplifier modules. 7 figs.

Ultrafast carrier thermalization and cooling dynamics in few-layer MoS2.

PubMed

Nie, Zhaogang; Long, Run; Sun, Linfeng; Huang, Chung-Che; Zhang, Jun; Xiong, Qihua; Hewak, Daniel W; Shen, Zexiang; Prezhdo, Oleg V; Loh, Zhi-Heng

2014-10-28

Femtosecond optical pump-probe spectroscopy with 10 fs visible pulses is employed to elucidate the ultrafast carrier dynamics of few-layer MoS2. A nonthermal carrier distribution is observed immediately following the photoexcitation of the A and B excitonic transitions by the ultrashort, broadband laser pulse. Carrier thermalization occurs within 20 fs and proceeds via both carrier-carrier and carrier-phonon scattering, as evidenced by the observed dependence of the thermalization time on the carrier density and the sample temperature. The n(-0.37 ± 0.03) scaling of the thermalization time with carrier density suggests that equilibration of the nonthermal carrier distribution occurs via non-Markovian quantum kinetics. Subsequent cooling of the hot Fermi-Dirac carrier distribution occurs on the ∼ 0.6 ps time scale via carrier-phonon scattering. Temperature- and fluence-dependence studies reveal the involvement of hot phonons in the carrier cooling process. Nonadiabatic ab initio molecular dynamics simulations, which predict carrier-carrier and carrier-phonon scattering time scales of 40 fs and 0.5 ps, respectively, lend support to the assignment of the observed carrier dynamics.

Ultrafast demagnetization enhancement in CoFeB/MgO/CoFeB magnetic tunneling junction driven by spin tunneling current.

PubMed

He, Wei; Zhu, Tao; Zhang, Xiang-Qun; Yang, Hai-Tao; Cheng, Zhao-Hua

2013-10-07

The laser-induced ultrafast demagnetization of CoFeB/MgO/CoFeB magnetic tunneling junction is exploited by time-resolved magneto-optical Kerr effect (TRMOKE) for both the parallel state (P state) and the antiparallel state (AP state) of the magnetizations between two magnetic layers. It was observed that the demagnetization time is shorter and the magnitude of demagnetization is larger in the AP state than those in the P state. These behaviors are attributed to the ultrafast spin transfer between two CoFeB layers via the tunneling of hot electrons through the MgO barrier. Our observation indicates that ultrafast demagnetization can be engineered by the hot electrons tunneling current. It opens the door to manipulate the ultrafast spin current in magnetic tunneling junctions.

Ultrafast amorphization in Ge(10)Sb(2)Te(13) thin film induced by single femtosecond laser pulse.

PubMed

Konishi, Mitsutaka; Santo, Hisashi; Hongo, Yuki; Tajima, Kazuyuki; Hosoi, Masaharu; Saiki, Toshiharu

2010-06-20

We demonstrate amorphization in a Ge(10)Sb(2)Te(13) (GST) thin film through a nonthermal process by femtosecond electronic excitation. Amorphous recording marks were formed by irradiation with a single femtosecond pulse, and were confirmed to be recrystallized by laser thermal annealing. Scanning electron microscope observations revealed that amorphization occurred below the melting temperature. We performed femtosecond pump-probe measurements to investigate the amorphization dynamics of a GST thin film. We found that the reflectivity dropped abruptly within 500fs after excitation by a single pulse and that a small change in the reflectivity occurred within 5ps of this drop.

Ultrafast lattice dynamics in lead selenide quantum dot induced by laser excitation

DOE PAGES

Wang, Xuan; Rahmani, Hamidreza; Zhou, Jun; ...

2016-10-10

We directly monitored the lattice dynamics in PbSe quantum dots induced by laser excitation using ultrafast electron di raction. The energy relaxation between the carriers and the lattice took place within 10 ps, showing no evidence of any signi cant phonon bottleneck e ect. Meanwhile, the lattice dilation exhibited some unusual features that could not be explained by the available mechanisms of photon- induced acoustic vibrations in semiconductors alone. The heat transport between the QDs and the substrate deviates signi cantly from Fourier's Law, which opens questions about the heat transfer under nonequilibrium conditions in nanoscale materials.

Ultrafast lattice dynamics in lead selenide quantum dot induced by laser excitation

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

Wang, Xuan; Rahmani, Hamidreza; Zhou, Jun

We directly monitored the lattice dynamics in PbSe quantum dots induced by laser excitation using ultrafast electron di raction. The energy relaxation between the carriers and the lattice took place within 10 ps, showing no evidence of any signi cant phonon bottleneck e ect. Meanwhile, the lattice dilation exhibited some unusual features that could not be explained by the available mechanisms of photon- induced acoustic vibrations in semiconductors alone. The heat transport between the QDs and the substrate deviates signi cantly from Fourier's Law, which opens questions about the heat transfer under nonequilibrium conditions in nanoscale materials.

The effect of solvent relaxation time constants on free energy gap law for ultrafast charge recombination following photoinduced charge separation.

PubMed

Mikhailova, Valentina A; Malykhin, Roman E; Ivanov, Anatoly I

2018-05-16

To elucidate the regularities inherent in the kinetics of ultrafast charge recombination following photoinduced charge separation in donor-acceptor dyads in solutions, the simulations of the kinetics have been performed within the stochastic multichannel point-transition model. Increasing the solvent relaxation time scales has been shown to strongly vary the dependence of the charge recombination rate constant on the free energy gap. In slow relaxing solvents the non-equilibrium charge recombination occurring in parallel with solvent relaxation is very effective so that the charge recombination terminates at the non-equilibrium stage. This results in a crucial difference between the free energy gap laws for the ultrafast charge recombination and the thermal charge transfer. For the thermal reactions the well-known Marcus bell-shaped dependence of the rate constant on the free energy gap is realized while for the ultrafast charge recombination only a descending branch is predicted in the whole area of the free energy gap exceeding 0.2 eV. From the available experimental data on the population kinetics of the second and first excited states for a series of Zn-porphyrin-imide dyads in toluene and tetrahydrofuran solutions, an effective rate constant of the charge recombination into the first excited state has been calculated. The obtained rate constant being very high is nearly invariable in the area of the charge recombination free energy gap from 0.2 to 0.6 eV that supports the theoretical prediction.

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

NASA Astrophysics Data System (ADS)

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

2016-10-01

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

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

PubMed Central

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

2016-01-01

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

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

PubMed

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

2016-10-20

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

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

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.

Ultrafast active control of UV light with plasmonic resonance on aluminum nanostripes

NASA Astrophysics Data System (ADS)

Wang, Kuidong; Li, Runze; Hsiao, Hui-Hsin; Chen, Long; Zhang, Haijuan; Chen, Jie

2018-05-01

Ultrafast active control of UV light with aluminum may become an efficient way for high-speed active UV devices. However, the nonlinear optical response of aluminum in the UV region is extremely small, which impedes the realization of the promising modulation depth on ultrafast control. Here, by using the surface plasmon resonance effect, we have achieved a 55-times enhancement in the modulation depth, as well as a short switching time of several picoseconds. Further investigation showed that such an enhancement mainly resulted from a two-order-of-magnitude boost in the response of the signal light to the lattice thermal variation at the plasmonic resonance condition. This improvement in the probing sensitivity could serve as an effective approach to resolve the dynamics of lattice vibrations in metals.

First-Principles Quantum Dynamics of Singlet Fission: Coherent versus Thermally Activated Mechanisms Governed by Molecular π Stacking

NASA Astrophysics Data System (ADS)

Tamura, Hiroyuki; Huix-Rotllant, Miquel; Burghardt, Irene; Olivier, Yoann; Beljonne, David

2015-09-01

Singlet excitons in π -stacked molecular crystals can split into two triplet excitons in a process called singlet fission that opens a route to carrier multiplication in photovoltaics. To resolve controversies about the mechanism of singlet fission, we have developed a first principles nonadiabatic quantum dynamical model that reveals the critical role of molecular stacking symmetry and provides a unified picture of coherent versus thermally activated singlet fission mechanisms in different acenes. The slip-stacked equilibrium packing structure of pentacene derivatives is found to enhance ultrafast singlet fission mediated by a coherent superexchange mechanism via higher-lying charge transfer states. By contrast, the electronic couplings for singlet fission strictly vanish at the C2 h symmetric equilibrium π stacking of rubrene. In this case, singlet fission is driven by excitations of symmetry-breaking intermolecular vibrations, rationalizing the experimentally observed temperature dependence. Design rules for optimal singlet fission materials therefore need to account for the interplay of molecular π -stacking symmetry and phonon-induced coherent or thermally activated mechanisms.

Nonthermal model for ultrafast laser-induced plasma generation around a plasmonic nanorod

NASA Astrophysics Data System (ADS)

Labouret, Timothée; Palpant, Bruno

2016-12-01

The excitation of plasmonic gold nanoparticles by ultrashort laser pulses can trigger interesting electron-based effects in biological media such as production of reactive oxygen species or cell membrane optoporation. In order to better understand the optical and thermal processes at play, we modeled the interaction of a subpicosecond, near-infrared laser pulse with a gold nanorod in water. A nonthermal model is used and compared to a simple two-temperature thermal approach. For both models, the computation of the transient optical response reveals strong plasmon damping. Electron emission from the metal into the water is also calculated in a specific way for each model. The dynamics of the resulting local plasma in water is assessed by a rate equation model. While both approaches provide similar results for the transient optical properties, the simple thermal one is unable to properly describe electron emission and plasma generation. The latter is shown to mostly originate from electron-electron thermionic emission and photoemission from the metal. Taking into account the transient optical response is mandatory to properly calculate both electron emission and local plasma dynamics in water.

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 bimetallic heterodimers are discussed in the last part of the review, demonstrating the existence of Fano interferences in the optical absorption of a gold nanoparticle under the influence of a nearby silver one.

Evidence for photo-induced monoclinic metallic VO{sub 2} under high pressure

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

Hsieh, Wen-Pin, E-mail: wphsieh@stanford.edu; Mao, Wendy L.; Department of Geological and Environmental Sciences, Stanford University, Stanford, California 94305

2014-01-13

We combine ultrafast pump-probe spectroscopy with a diamond-anvil cell to decouple the insulator-metal electronic transition from the lattice symmetry changing structural transition in the archetypal strongly correlated material vanadium dioxide. Coherent phonon spectroscopy enables tracking of the photo-excited phonon vibrational frequencies of the low temperature, monoclinic (M{sub 1})-insulating phase that transforms into the metallic, tetragonal rutile structured phase at high temperature or via non-thermal photo-excitations. We find that in contrast with ambient pressure experiments where strong photo-excitation promptly induces the electronic transition along with changes in the lattice symmetry, at high pressure, the coherent phonons of the monoclinic (M{sub 1})more » phase are still clearly observed upon the photo-driven phase transition to a metallic state. These results demonstrate the possibility of synthesizing and studying transient phases under extreme conditions.« less

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.

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

Design, fabrication, and experimental characterization of plasmonic photoconductive terahertz emitters.

PubMed

Berry, Christopher; Hashemi, Mohammad Reza; Unlu, Mehmet; Jarrahi, Mona

2013-07-08

In this video article we present a detailed demonstration of a highly efficient method for generating terahertz waves. Our technique is based on photoconduction, which has been one of the most commonly used techniques for terahertz generation (1-8). Terahertz generation in a photoconductive emitter is achieved by pumping an ultrafast photoconductor with a pulsed or heterodyned laser illumination. The induced photocurrent, which follows the envelope of the pump laser, is routed to a terahertz radiating antenna connected to the photoconductor contact electrodes to generate terahertz radiation. Although the quantum efficiency of a photoconductive emitter can theoretically reach 100%, the relatively long transport path lengths of photo-generated carriers to the contact electrodes of conventional photoconductors have severely limited their quantum efficiency. Additionally, the carrier screening effect and thermal breakdown strictly limit the maximum output power of conventional photoconductive terahertz sources. To address the quantum efficiency limitations of conventional photoconductive terahertz emitters, we have developed a new photoconductive emitter concept which incorporates a plasmonic contact electrode configuration to offer high quantum-efficiency and ultrafast operation simultaneously. By using nano-scale plasmonic contact electrodes, we significantly reduce the average photo-generated carrier transport path to photoconductor contact electrodes compared to conventional photoconductors (9). Our method also allows increasing photoconductor active area without a considerable increase in the capacitive loading to the antenna, boosting the maximum terahertz radiation power by preventing the carrier screening effect and thermal breakdown at high optical pump powers. By incorporating plasmonic contact electrodes, we demonstrate enhancing the optical-to-terahertz power conversion efficiency of a conventional photoconductive terahertz emitter by a factor of 50 (10).

Progress in ultrafast laser processing and future prospects

NASA Astrophysics Data System (ADS)

Sugioka, Koji

2017-03-01

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

Phase transformation pathways of ultrafast-laser-irradiated Ln2O3 (Ln =Er -Lu )

NASA Astrophysics Data System (ADS)

Rittman, Dylan R.; Tracy, Cameron L.; Chen, Chien-Hung; Solomon, Jonathan M.; Asta, Mark; Mao, Wendy L.; Yalisove, Steven M.; Ewing, Rodney C.

2018-01-01

Ultrafast laser irradiation causes intense electronic excitations in materials, leading to transient high temperatures and pressures. Here, we show that ultrafast laser irradiation drives an irreversible cubic-to-monoclinic phase transformation in Ln2O3 (Ln =Er -Lu ), and explore the mechanism by which the phase transformation occurs. A combination of grazing incidence x-ray diffraction and transmission electron microscopy are used to determine the magnitude and depth-dependence of the phase transformation, respectively. Although all compositions undergo the same transformation, their transformation mechanisms differ. The transformation is pressure-driven for Ln =Tm -Lu , consistent with the material's phase behavior under equilibrium conditions. However, the transformation is thermally driven for Ln =Er , revealing that the nonequilibrium conditions of ultrafast laser irradiation can lead to novel transformation pathways. Ab initio molecular-dynamics simulations are used to examine the atomic-scale effects of electronic excitation, showing the production of oxygen Frenkel pairs and the migration of interstitial oxygen to tetrahedrally coordinated constitutional vacancy sites, the first step in a defect-driven phase transformation.

Phase transformation pathways of ultrafast-laser-irradiated Ln 2 O 3 ( Ln = Er – Lu )

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

Rittman, Dylan R.; Tracy, Cameron L.; Chen, Chien-Hung

Ultrafast laser irradiation causes intense electronic excitations in materials, leading to transient high temperatures and pressures. Here, we show that ultrafast laser irradiation drives an irreversible cubic-to-monoclinic phase transformation in Ln 2O 3 ( Ln = Er – Lu ) , and explore the mechanism by which the phase transformation occurs. A combination of grazing incidence x-ray diffraction and transmission electron microscopy are used to determine the magnitude and depth-dependence of the phase transformation, respectively. Although all compositions undergo the same transformation, their transformation mechanisms differ. The transformation is pressure-driven for Ln = Tm – Lu , consistent with themore » material's phase behavior under equilibrium conditions. However, the transformation is thermally driven for Ln = Er , revealing that the nonequilibrium conditions of ultrafast laser irradiation can lead to novel transformation pathways. Ab initio molecular-dynamics simulations are used to examine the atomic-scale effects of electronic excitation, showing the production of oxygen Frenkel pairs and the migration of interstitial oxygen to tetrahedrally coordinated constitutional vacancy sites, the first step in a defect-driven phase transformation.« less

Phase transformation pathways of ultrafast-laser-irradiated Ln 2 O 3 ( Ln = Er – Lu )

DOE PAGES

Rittman, Dylan R.; Tracy, Cameron L.; Chen, Chien-Hung; ...

2018-01-10

Ultrafast laser irradiation causes intense electronic excitations in materials, leading to transient high temperatures and pressures. Here, we show that ultrafast laser irradiation drives an irreversible cubic-to-monoclinic phase transformation in Ln 2O 3 ( Ln = Er – Lu ) , and explore the mechanism by which the phase transformation occurs. A combination of grazing incidence x-ray diffraction and transmission electron microscopy are used to determine the magnitude and depth-dependence of the phase transformation, respectively. Although all compositions undergo the same transformation, their transformation mechanisms differ. The transformation is pressure-driven for Ln = Tm – Lu , consistent with themore » material's phase behavior under equilibrium conditions. However, the transformation is thermally driven for Ln = Er , revealing that the nonequilibrium conditions of ultrafast laser irradiation can lead to novel transformation pathways. Ab initio molecular-dynamics simulations are used to examine the atomic-scale effects of electronic excitation, showing the production of oxygen Frenkel pairs and the migration of interstitial oxygen to tetrahedrally coordinated constitutional vacancy sites, the first step in a defect-driven phase transformation.« less

Case study on the dynamics of ultrafast laser heating and ablation of gold thin films by ultrafast pump-probe reflectometry and ellipsometry

NASA Astrophysics Data System (ADS)

Pflug, T.; Wang, J.; Olbrich, M.; Frank, M.; Horn, A.

2018-02-01

To increase the comprehension of ultrafast laser ablation, the ablation process has to be portrayed with sufficient temporal resolution. For example, the temporal modification of the complex refractive index {\\tilde{n}} and the relative reflectance of a sample material after irradiation with ultrafast single-pulsed laser radiation can be measured with a pump-probe setup. This work describes the construction and validation of a pump-probe setup enabling spatially, temporally, and spectroscopically resolved Brewster angle microscopy, reflectometry, ellipsometry, and shadow photography. First pump-probe reflectometry and ellipsometry measurements are performed on gold at λ _{probe}= 440 nm and three fluences of the single-pulsed pump radiation at λ _{pump}= 800 nm generating no, gentle, and strong ablation. The relative reflectance overall increases at no and gentle ablation. At strong ablation, the relative reflectance locally decreases, presumable caused by emitted thermal electrons, ballistic electrons, and ablating material. The refractive index n is slightly decreasing after excitation, while the extinction coefficient k is increasing.

Hard-X-Ray-Induced Multistep Ultrafast Dissociation

NASA Astrophysics Data System (ADS)

Travnikova, Oksana; Marchenko, Tatiana; Goldsztejn, Gildas; Jänkälä, Kari; Sisourat, Nicolas; Carniato, Stéphane; Guillemin, Renaud; Journel, Loïc; Céolin, Denis; Püttner, Ralph; Iwayama, Hiroshi; Shigemasa, Eiji; Piancastelli, Maria Novella; Simon, Marc

2016-05-01

Creation of deep core holes with very short (τ ≤1 fs ) lifetimes triggers a chain of relaxation events leading to extensive nuclear dynamics on a few-femtosecond time scale. Here we demonstrate a general multistep ultrafast dissociation on an example of HCl following Cl 1 s →σ* excitation. Intermediate states with one or multiple holes in the shallower core electron shells are generated in the course of the decay cascades. The repulsive character and large gradients of the potential energy surfaces of these intermediates enable ultrafast fragmentation after the absorption of a hard x-ray photon.

Sub-nanometre resolution of atomic motion during electronic excitation in phase-change materials.

PubMed

Mitrofanov, Kirill V; Fons, Paul; Makino, Kotaro; Terashima, Ryo; Shimada, Toru; Kolobov, Alexander V; Tominaga, Junji; Bragaglia, Valeria; Giussani, Alessandro; Calarco, Raffaella; Riechert, Henning; Sato, Takahiro; Katayama, Tetsuo; Ogawa, Kanade; Togashi, Tadashi; Yabashi, Makina; Wall, Simon; Brewe, Dale; Hase, Muneaki

2016-02-12

Phase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived (>100 ps) transient metastable state of Ge2Sb2Te5 with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structure experiment confirms the existence of an intermediate state with disordered bonds. This newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit, and improved energy efficiency and reliability of phase-change memory technologies.

Sub-nanometre resolution of atomic motion during electronic excitation in phase-change materials

DOE PAGES

Mitrofanov, Kirill V.; Fons, Paul; Makino, Kotaro; ...

2016-02-12

Phase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived (>100 ps) transient metastable state of Ge 2Sb 2Te 5 with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structuremore » experiment confirms the existence of an intermediate state with disordered bonds. Furthermore, this newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit, and improved energy efficiency and reliability of phase-change memory technologies.« less

Ultrafast cavitation induced by an X-ray laser in water drops

NASA Astrophysics Data System (ADS)

Stan, Claudiu; Willmott, Philip; Stone, Howard; Koglin, Jason; Liang, Mengning; Aquila, Andrew; Robinson, Joseph; Gumerlock, Karl; Blaj, Gabriel; Sierra, Raymond; Boutet, Sebastien; Guillet, Serge; Curtis, Robin; Vetter, Sharon; Loos, Henrik; Turner, James; Decker, Franz-Josef

2016-11-01

Cavitation in pure water is determined by an intrinsic heterogeneous cavitation mechanism, which prevents in general the experimental generation of large tensions (negative pressures) in bulk liquid water. We developed an ultrafast decompression technique, based on the reflection of shock waves generated by an X-ray laser inside liquid drops, to stretch liquids to large negative pressures in a few nanoseconds. Using this method, we observed cavitation in liquid water at pressures below -100 MPa. These large tensions exceed significantly those achieved previously, mainly due to the ultrafast decompression. The decompression induced by shock waves generated by an X-ray laser is rapid enough to continue to stretch the liquid phase after the heterogeneous cavitation occurs in water, despite the rapid growth of cavitation nanobubbles. We developed a nucleation-and-growth hydrodynamic cavitation model that explains our results and estimates the concentration of heterogeneous cavitation nuclei in water.

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.

Strong field acceleration and steering of ultrafast electron pulses from a sharp metallic nanotip.

PubMed

Park, Doo Jae; Piglosiewicz, Bjoern; Schmidt, Slawa; Kollmann, Heiko; Mascheck, Manfred; Lienau, Christoph

2012-12-14

We report a strong, laser-field induced modification of the propagation direction of ultrashort electron pulses emitted from nanometer-sized gold tapers. Angle-resolved kinetic energy spectra of electrons emitted from such tips are recorded using ultrafast near-infrared light pulses of variable wavelength and intensity for excitation. For sufficiently long wavelengths, we observe a pronounced strong-field acceleration of electrons within the field gradient at the taper apex. We find a distinct narrowing of the emission cone angle of the fastest electrons. We ascribe this to the field-induced steering of subcycle electrons as opposed to the diverging emission of quiver electrons. Our findings are corroborated by simulations based on a modified Simpleman model incorporating the curved, vectorial field gradient in the vicinity of the tip. Our results indicate new pathways for designing highly directional nanometer-sized ultrafast electron sources.

Ultrafast saturable absorption in TiS2 induced by non-equilibrium electrons and the generation of a femtosecond mode-locked laser.

PubMed

Tian, Xiangling; Wei, Rongfei; Liu, Meng; Zhu, Chunhui; Luo, Zhichao; Wang, Fengqiu; Qiu, Jianrong

2018-05-24

Non-equilibrium electrons induced by ultrafast laser excitation in a correlated electron material can disturb the Fermi energy as well as optical nonlinearity. Here, non-equilibrium electrons translate a semiconductor TiS2 material into a plasma to generate broad band nonlinear optical saturable absorption with a sub-picosecond recovery time of ∼768 fs (corresponding to modulation frequencies over 1.3 THz) and a modulation response up to ∼145%. Based on this optical nonlinear modulator, a stable femtosecond mode-locked pulse with a pulse duration of ∼402 fs and a pulse train with a period of ∼175.5 ns is observed in the all-optical system. The findings indicate that non-equilibrium electrons can promote a TiS2-based saturable absorber to be an ultrafast switch for a femtosecond pulse output.

Ultrafast Surface-Enhanced Raman Probing of the Role of Hot Electrons in Plasmon-Driven Chemistry.

PubMed

Brandt, Nathaniel C; Keller, Emily L; Frontiera, Renee R

2016-08-18

Hot electrons generated through plasmonic excitations in metal nanostructures show great promise for efficiently driving chemical reactions with light. However, the lifetime, yield, and mechanism of action of plasmon-generated hot electrons involved in a given photocatalytic process are not well understood. Here, we develop ultrafast surface-enhanced Raman scattering (SERS) as a direct probe of plasmon-molecule interactions in the plasmon-catalyzed dimerization of 4-nitrobenzenethiol to p,p'-dimercaptoazobenzene. Ultrafast SERS probing of these molecular reporters in plasmonic hot spots reveals transient Fano resonances, which we attribute to near-field coupling of Stokes-shifted photons to hot electron-driven metal photoluminescence. Surprisingly, we find that hot spots that yield more photoluminescence are much more likely to drive the reaction, which indirectly proves that plasmon-generated hot electrons induce the photochemistry. These ultrafast SERS results provide insight into the relative reactivity of different plasmonic hot spot environments and quantify the ultrafast lifetime of hot electrons involved in plasmon-driven chemistry.

Vibronically coherent ultrafast triplet-pair formation and subsequent thermally activated dissociation control efficient endothermic singlet fission

NASA Astrophysics Data System (ADS)

Stern, Hannah L.; Cheminal, Alexandre; Yost, Shane R.; Broch, Katharina; Bayliss, Sam L.; Chen, Kai; Tabachnyk, Maxim; Thorley, Karl; Greenham, Neil; Hodgkiss, Justin M.; Anthony, John; Head-Gordon, Martin; Musser, Andrew J.; Rao, Akshay; Friend, Richard H.

2017-12-01

Singlet exciton fission (SF), the conversion of one spin-singlet exciton (S1) into two spin-triplet excitons (T1), could provide a means to overcome the Shockley-Queisser limit in photovoltaics. SF as measured by the decay of S1 has been shown to occur efficiently and independently of temperature, even when the energy of S1 is as much as 200 meV less than that of 2T1. Here we study films of triisopropylsilyltetracene using transient optical spectroscopy and show that the triplet pair state (TT), which has been proposed to mediate singlet fission, forms on ultrafast timescales (in 300 fs) and that its formation is mediated by the strong coupling of electronic and vibrational degrees of freedom. This is followed by a slower loss of singlet character as the excitation evolves to become only TT. We observe the TT to be thermally dissociated on 10-100 ns timescales to form free triplets. This provides a model for 'temperature-independent' efficient TT formation and thermally activated TT separation.

Femtosecond dynamics in hydrogen-bonded solvents

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

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

1993-09-01

We present results on the ultrafast dynamics of pure hydrogen-bonding solvents, obtained using femtosecond Fourier-transform optical-heterodyne-detected, Raman-induced Kerr effect spectroscopy. Solvent systems we have studied include the formamides, water, ethylene glycol, and acetic acid. Inertial and diffusive motions are clearly resolved. We comment on the effect that such ultrafast solvent motions have on chemical reactions in solution.

Reversible ultrafast melting in bulk CdSe

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

Wu, Wenzhi; Department of Mechanical Engineering, The University of Texas at Austin, Austin, Texas 78712; He, Feng

2016-02-07

In this work, transient reflectivity changes in bulk CdSe have been measured with two-color femtosecond pump-probe spectroscopy under a wide range of pump fluences. Three regions of reflectivity change with pump fluences have been consistently revealed for excited carrier density, coherent phonon amplitude, and lattice temperature. For laser fluences from 13 to 19.3 mJ/cm{sup 2}, ultrafast melting happens in first several picoseconds. This melting process is purely thermal and reversible. A complete phase transformation in bulk CdSe may be reached when the absorbed laser energy is localized long enough, as observed in nanocrystalline CdSe.

Effective thermal and mechanical properties of polycrystalline diamond films

NASA Astrophysics Data System (ADS)

Cheng, Hao-Yu; Yang, Chi-Yuan; Yang, Li-Chueh; Peng, Kun-Cheng; Chia, Chih-Ta; Liu, Shiu-Jen; Lin, I.-Nan; Lin, Kung-Hsuan

2018-04-01

Polycrystalline diamond films were demonstrated as good candidates for electron field emitters, and their mechanical/thermal properties should thus be considered for real devices. We utilized ultrafast optical techniques to investigate the phonon dynamics of several polycrystalline diamond films, prepared by microwave plasma enhanced chemical vapor deposition. The mechanical properties (longitudinal acoustic velocity) and thermal conductivities of diamond films were evaluated from the coherent and incoherent phonon dynamics, respectively. Ultrananocrystalline diamond films were grown using a CH4 (2%)/Ar plasma, while microcrystalline diamond films were grown using a CH4 (2%)/H2 plasma. The ultrananocrystalline diamond film (with a grain size of several nanometers) possesses low acoustic velocity (14.5 nm/ps) and low thermal conductivity (3.17 W/m K) compared with other kinds of diamond films. The acoustic velocity of diamond films increased abruptly to nearly the same as that of natural diamond and remained there when the rod-shaped diamond grains were induced due to the incorporation of H2 in the growth plasma (CH4/Ar). The thermal conductivities of the materials increased monotonously with increasing incorporation of H2 in the growth plasma (CH4/Ar). The thermal conductivity of 25.6 W/m K was attained for nanocrystalline diamond films containing spherical diamond grains (with a size of several tens of nanometers). Compared with single crystalline diamond, the low thermal conductivity of polycrystalline films results from phonon scattering at the interfaces of grains and amorphous carbon in the boundary phases.

Dynamic Optoelectronic Properties in Perovskite Oxide Thin Films Measured with Ultrafast Transient Absorption & Reflectance Spectroscopy

NASA Astrophysics Data System (ADS)

Smolin, Sergey Y.

Ultrafast transient absorption and reflectance spectroscopy are foundational techniques for studying photoexcited carrier recombination mechanisms, lifetimes, and charge transfer rates. Because quantifying photoexcited carrier dynamics is central to the intelligent design and improvement of many solid state devices, these transient optical techniques have been applied to a wide range of semiconductors. However, despite their promise, interpretation of transient absorption and reflectance data is not always straightforward and often relies on assumptions of physical processes, especially with respect to the influence of heating. Studying the material space of perovskite oxides, the careful collection, interpretation, and analysis of ultrafast data is presented here as a guide for future research into novel semiconductors. Perovskite oxides are a class of transition metal oxides with the chemical structure ABO3. Although traditionally studied for their diverse physical, electronic, and magnetic properties, perovskite oxides have gained recent research attention as novel candidates for light harvesting applications. Indeed, strong tunable absorption, unique interfacial properties, and vast chemical flexibility make perovskite oxides a promising photoactive material system. However, there is limited research characterizing dynamic optoelectronic properties, such as recombination lifetimes, which are critical to know in the design of any light-harvesting device. In this thesis, ultrafast transient absorption and reflectance spectroscopy was used to understand these dynamic optoelectronic properties in highquality, thin (<50 nm) perovskite oxide films grown by molecular beam epitaxy. Starting with epitaxial LaFeO3 (LFO) grown on (LaAlO 3)0.3(Sr2AlTaO6)0.7 (LSAT), transient absorption spectroscopy reveals two photoinduced absorption features at the band gap of LFO at 2.4 eV and at the higher energy absorption edge at 3.5 eV. Using a combination of temperature-dependent, variable-angle spectroscopic ellipsometry and time-resolved ultrafast optical spectroscopy on a type I heterostructure, we clarify thermal and electronic contributions to spectral transients in LaFeO3. Upon comparison to thermally-derived static spectra of LaFeO3, we find that thermal contributions dominate the transient absorption and reflectance spectra above the band gap. A transient photoinduced absorption feature below the band gap at 1.9 eV is not reproduced in the thermally derived spectra and has significantly longer decay kinetics from the thermallyinduced features; therefore, this long lived photoinduced absorption is likely derived, at least partially, from photoexcited carriers with lifetimes much longer than 3 nanoseconds. LaFeO3 has a wide band gap of 2.4 eV but its absorption can be decreased with chemical substitution of Sr for Fe to make it more suitable for various applications. This type of A-site substitution is a common route to change static optical absorption in perovskite oxides, but there are no systematic studies looking at how A-site substitution changes dynamic optoelectronic properties. To understand the relationship between composition and static and dynamic optical properties we worked with the model system of La1-xSrxFeO 3-delta epitaxial films grown on LSAT, uncovering the effects of A-site cation substitution and oxygen stoichiometry. Variable-angle spectroscopic ellipsometry was used to measure static optical properties, revealing a linear increase in absorption coefficient at 1.25 eV and a red-shifting of the optical absorption edge with increasing Sr fraction. The absorption spectra can be similarly tuned through the introduction of oxygen vacancies, indicating the critical role that nominal Fe valence plays in optical absorption. Dynamic optoelectronic properties were studied with ultrafast transient reflectance spectroscopy with broadband visible (1.6 eV to 4 eV) and near-infrared (0.9 eV to 1.5 eV) probes. The sign of the reflectance change in the near-infrared region in LSFO is indicative of carrier bandfilling of newly created electronic states by photoexcited carriers. Moreover, we find that similar transient spectral trends can be induced with A-site substitution or through oxygen vacancies, which is a surprising result. Probing the near-infrared region reveals similar nanosecond (1-3 ns) photoexcited carrier lifetimes for oxygen deficient and stoichiometric films. These results demonstrate that while the static optical absorption is strongly dependent on nominal Fe valence tuned through cation or anion stoichiometry, oxygen vacancies do not appear to play a significantly detrimental role in long lived recombination kinetics. Although this thesis represents one of the first comprehensive studies using broad band transient absorption and reflectance spectroscopy to study dynamic optoelectronic phenomena in perovskite oxides, it can also serve as a guide for the implementation and interpretation of ultrafast spectroscopy in other material systems. Moreover, the ultrafast work on perovskite oxides indicates that these materials have long nanosecond lifetimes required for light harvesting devices and should be investigated further.

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.

Ultrafast switching of valence and generation of coherent acoustic phonons in semiconducting rare-earth monosulfides

NASA Astrophysics Data System (ADS)

Punpongjareorn, Napat; He, Xing; Tang, Zhongjia; Guloy, Arnold M.; Yang, Ding-Shyue

2017-08-01

We report on the ultrafast carrier dynamics and generation of coherent acoustic phonons in YbS, a semiconducting rare-earth monochalcogenide, using two-color pump-probe reflectivity. Compared to the carrier relaxation processes and lifetimes of conventional semiconductors, recombination of photoexcited electrons with holes in localized f orbitals is found to take place rapidly with a density-independent time constant of <500 fs in YbS. Such carrier annihilation signifies the unique and ultrafast nature of valence restoration of ytterbium ions after femtosecond photoexcitation switching. Following transfer of the absorbed energy to the lattice, coherent acoustic phonons emerge on the picosecond timescale as a result of the thermal strain in the photoexcited region. By analyzing the electronic and structural dynamics, we obtain the physical properties of YbS including its two-photon absorption and thermooptic coefficients, the period and decay time of the coherent oscillation, and the sound velocity.

Dynamic diffraction effects and coherent breathing oscillations in ultrafast electron diffraction in layered 1T-TaSeTe

PubMed Central

Wei, Linlin; Sun, Shuaishuai; Guo, Cong; Li, Zhongwen; Sun, Kai; Liu, Yu; Lu, Wenjian; Sun, Yuping; Tian, Huanfang; Yang, Huaixin; Li, Jianqi

2017-01-01

Anisotropic lattice movements due to the difference between intralayer and interlayer bonding are observed in the layered transition-metal dichalcogenide 1T-TaSeTe following femtosecond laser pulse excitation. Our ultrafast electron diffraction investigations using 4D-transmission electron microscopy (4D-TEM) clearly reveal that the intensity of Bragg reflection spots often changes remarkably due to the dynamic diffraction effects and anisotropic lattice movement. Importantly, the temporal diffracted intensity from a specific crystallographic plane depends on the deviation parameter s, which is commonly used in the theoretical study of diffraction intensity. Herein, we report on lattice thermalization and structural oscillations in layered 1T-TaSeTe, analyzed by dynamic diffraction theory. Ultrafast alterations of satellite spots arising from the charge density wave in the present system are also briefly discussed. PMID:28470025

Measurements of ultrafast spin-profiles and spin-diffusion properties in the domain wall area at a metal/ferromagnetic film interface.

PubMed

Sant, T; Ksenzov, D; Capotondi, F; Pedersoli, E; Manfredda, M; Kiskinova, M; Zabel, H; Kläui, M; Lüning, J; Pietsch, U; Gutt, C

2017-11-08

Exciting a ferromagnetic material with an ultrashort IR laser pulse is known to induce spin dynamics by heating the spin system and by ultrafast spin diffusion processes. Here, we report on measurements of spin-profiles and spin diffusion properties in the vicinity of domain walls in the interface region between a metallic Al layer and a ferromagnetic Co/Pd thin film upon IR excitation. We followed the ultrafast temporal evolution by means of an ultrafast resonant magnetic scattering experiment in surface scattering geometry, which enables us to exploit the evolution of the domain network within a 1/e distance of 3 nm to 5 nm from the Al/FM film interface. We observe a magnetization-reversal close to the domain wall boundaries that becomes more pronounced closer to the Al/FM film interface. This magnetization-reversal is driven by the different transport properties of majority and minority carriers through a magnetically disordered domain network. Its finite lateral extension has allowed us to measure the ultrafast spin-diffusion coefficients and ultrafast spin velocities for majority and minority carriers upon IR excitation.

Femtosecond laser melting of silver nanoparticles: comparison of model simulations and experimental results

NASA Astrophysics Data System (ADS)

Cheng, Chung-Wei; Chang, Chin-Lun; Chen, Jinn-Kuen; Wang, Ben

2018-05-01

Ultrafast laser-induced melting of silver nanoparticles (NPs) using a femtosecond laser pulse is investigated both theoretically and experimentally. The sintered Ag structure fabricated from printed Ag NP ink using femtosecond laser (1064 nm, 300 fs) irradiation is experimentally studied. A two-temperature model with dynamic optical properties and particle size effects on the melting temperature of Ag NPs is considered. The rapid phase change model is incorporated to simulate the Ag NPs' ultrafast laser-induced melting process, and a multi-shot melting threshold fluence predicted from the simulated single-shot melting threshold is developed.

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.

Multiphoton manipulations of enzymatic photoactivity in aspartate aminotransferase.

PubMed

Hill, Melissa P; Freer, Lucy H; Vang, Mai C; Carroll, Elizabeth C; Larsen, Delmar S

2011-04-21

The aspartate aminotransferase (AAT) enzyme utilizes the chromophoric pyridoxal 5'-phosphate (PLP) cofactor to facilitate the transamination of amino acids. Recently, we demonstrated that, upon exposure to blue light, PLP forms a reactive triplet state that rapidly (in microseconds) generates the high-energy quinonoid intermediate when bound to PLP-dependent enzymes [J. Am. Chem. Soc.2010, 132 (47), 16953-16961]. This increases the net catalytic activity (k(cat)) of AAT, since formation of the quinonoid is partially rate limiting via the thermally activated enzymatic pathway. The magnitude of observed photoenhancement initially scales linearly with pump fluence; however when a critical threshold is exceeded, the photoactivity saturates and is even suppressed at greater excitation fluences. The photodynamic mechanisms associated with this suppression behavior are characterized with the use of ultrafast multipulse pump-dump-probe and pump-repump-probe transient absorption techniques in combination with complementary two-color, steady-state excitation assays. Via multistate kinetic modeling of the transient ultrafast data and the steady-state assay data, the nonmonotonic incident power dependence of the photoactivty in AAT is decomposed into contributions from high-intensity dumping of the excited singlet state and repumping of the excited triplet state with induces the repopulation of the ground state via rapid intersystem crossing in the higher-lying triplet electronic manifold.

Ultrafast Laser-Based Spectroscopy and Sensing: Applications in LIBS, CARS, and THz Spectroscopy

PubMed Central

Leahy-Hoppa, Megan R.; Miragliotta, Joseph; Osiander, Robert; Burnett, Jennifer; Dikmelik, Yamac; McEnnis, Caroline; Spicer, James B.

2010-01-01

Ultrafast pulsed lasers find application in a range of spectroscopy and sensing techniques including laser induced breakdown spectroscopy (LIBS), coherent Raman spectroscopy, and terahertz (THz) spectroscopy. Whether based on absorption or emission processes, the characteristics of these techniques are heavily influenced by the use of ultrafast pulses in the signal generation process. Depending on the energy of the pulses used, the essential laser interaction process can primarily involve lattice vibrations, molecular rotations, or a combination of excited states produced by laser heating. While some of these techniques are currently confined to sensing at close ranges, others can be implemented for remote spectroscopic sensing owing principally to the laser pulse duration. We present a review of ultrafast laser-based spectroscopy techniques and discuss the use of these techniques to current and potential chemical and environmental sensing applications. PMID:22399883

Growth of ferroelectric Ba{sub 0.8}Sr{sub 0.2}TiO{sub 3} epitaxial films by ultraviolet pulsed laser irradiation of chemical solution derived precursor layers

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

Queraltó, A.; Pérez del Pino, A., E-mail: aperez@icmab.es; Mata, M. de la

2015-06-29

Highly crystalline epitaxial Ba{sub 0.8}Sr{sub 0.2}TiO{sub 3} (BST) thin-films are grown on (001)-oriented LaNiO{sub 3}-buffered LaAlO{sub 3} substrates by pulsed laser irradiation of solution derived barium-zirconium-titanium precursor layers using a UV Nd:YAG laser source at atmospheric conditions. The structural analyses of the obtained films, studied by X-ray diffractometry and transmission electron microscopy, demonstrate that laser processing allows the growth of tens of nm-thick BST epitaxial films with crystalline structure similar to that of films obtained through conventional thermal annealing methods. However, the fast pulsed nature of the laser employed leads to crystallization kinetic evolution orders of magnitude faster than inmore » thermal treatments. The combination of specific photothermal and photochemical mechanisms is the main responsible for the ultrafast epitaxial laser-induced crystallization. Piezoresponse microscopy measurements demonstrate equivalent ferroelectric behavior in laser and thermally annealed films, being the piezoelectric constant ∼25 pm V{sup −1}.« less

Ultrafast dynamics of hard tissue ablation using fs-lasers.

PubMed

Domke, Matthias; Wick, Sebastian; Laible, Maike; Rapp, Stephan; Huber, Heinz P; Sroka, Ronald

2018-05-29

Several studies on hard tissue laser ablation demonstrated that ultrafast lasers enable precise material removal without thermal side effects. Although the principle ablation mechanisms have been thoroughly investigated, there are still open questions regarding the influence of material properties on transient dynamics. In this investigation, we applied pump-probe microscopy to record ablation dynamics of biomaterials with different tensile strengths (dentin, chicken bone, gallstone, kidney stones) at delay times between 1 ps and 10 μs. Transient reflectivity changes, pressure and shock wave velocities, and elastic constants were determined. The result revealed that absorption and excitation show the typical well-known transient behaviour of dielectric materials. We observed for all samples a photomechanical laser ablation process, where ultrafast expansion of the excited volume generates pressure waves leading to fragmentation around the excited region. Additionally, we identified tensile-strength-related differences in the size of ablated craters and ejected particles. The elastic constants derived were in agreement with literature values. In conclusion, pressure-wave-assisted material removal seems to be a general mechanism for hard tissue ablation with ultrafast lasers. This photomechanical process increases ablation efficiency and removes heated material, thus ultrafast laser ablation is of interest for clinical application where heating of the tissue must be avoided. This article is protected by copyright. All rights reserved. This article is protected by copyright. All rights reserved.

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.

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.

Enhanced generation and anisotropic Coulomb scattering of hot electrons in an ultra-broadband plasmonic nanopatch metasurface.

PubMed

Sykes, Matthew E; Stewart, Jon W; Akselrod, Gleb M; Kong, Xiang-Tian; Wang, Zhiming; Gosztola, David J; Martinson, Alex B F; Rosenmann, Daniel; Mikkelsen, Maiken H; Govorov, Alexander O; Wiederrecht, Gary P

2017-10-17

The creation of energetic electrons through plasmon excitation of nanostructures before thermalization has been proposed for a wide number of applications in optical energy conversion and ultrafast nanophotonics. However, the use of "nonthermal" electrons is primarily limited by both a low generation efficiency and their ultrafast decay. We report experimental and theoretical results on the use of broadband plasmonic nanopatch metasurfaces comprising a gold substrate coupled to silver nanocubes that produce large concentrations of hot electrons, which we measure using transient absorption spectroscopy. We find evidence for three subpopulations of nonthermal carriers, which we propose arise from anisotropic electron-electron scattering within sp-bands near the Fermi surface. The bimetallic character of the metasurface strongly impacts the physics, with dissipation occurring primarily in the gold, whereas the quantum process of hot electron generation takes place in both components. Our calculations show that the choice of geometry and materials is crucial for producing strong ultrafast nonthermal electron components.The creation of energetic electrons through plasmon excitation has implications in optical energy conversion and ultrafast nanophotonics. Here, the authors find evidence for three subpopulations of nonthermal carriers which arise from anisotropic electron-electron scattering near the Fermi surface.

Single-shot ultrafast tomographic imaging by spectral multiplexing

NASA Astrophysics Data System (ADS)

Matlis, N. H.; Axley, A.; Leemans, W. P.

2012-10-01

Computed tomography has profoundly impacted science, medicine and technology by using projection measurements scanned over multiple angles to permit cross-sectional imaging of an object. The application of computed tomography to moving or dynamically varying objects, however, has been limited by the temporal resolution of the technique, which is set by the time required to complete the scan. For objects that vary on ultrafast timescales, traditional scanning methods are not an option. Here we present a non-scanning method capable of resolving structure on femtosecond timescales by using spectral multiplexing of a single laser beam to perform tomographic imaging over a continuous range of angles simultaneously. We use this technique to demonstrate the first single-shot ultrafast computed tomography reconstructions and obtain previously inaccessible structure and position information for laser-induced plasma filaments. This development enables real-time tomographic imaging for ultrafast science, and offers a potential solution to the challenging problem of imaging through scattering surfaces.

Low damage electrical modification of 4H-SiC via ultrafast laser irradiation

NASA Astrophysics Data System (ADS)

Ahn, Minhyung; Cahyadi, Rico; Wendorf, Joseph; Bowen, Willie; Torralva, Ben; Yalisove, Steven; Phillips, Jamie

2018-04-01

The electrical properties of 4H-SiC under ultrafast laser irradiation in the low fluence regime (<0.50 J/cm2) are presented. The appearance of high spatial frequency laser induced periodic surface structures is observed at a fluence near 0.25 J/cm2 and above, with variability in environments like in air, nitrogen, and a vacuum. In addition to the formation of periodic surface structures, ultrafast laser irradiation results in possible surface oxidation and amorphization of the material. Lateral conductance exhibits orders of magnitude increase, which is attributed to either surface conduction or modification of electrical contact properties, depending on the initial material conductivity. Schottky barrier formation on ultrafast laser irradiated 4H-SiC shows an increase in the barrier height, an increase in the ideality factor, and sub-bandgap photovoltaic responses, suggesting the formation of photo-active point defects. The results suggest that the ultrafast laser irradiation technique provides a means of engineering spatially localized structural and electronic modification of wide bandgap materials such as 4H-SiC with relatively low surface damage via low temperature processing.

Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals.

PubMed

Cherukara, Mathew J; Sasikumar, Kiran; Cha, Wonsuk; Narayanan, Badri; Leake, Steven J; Dufresne, Eric M; Peterka, Tom; McNulty, Ian; Wen, Haidan; Sankaranarayanan, Subramanian K R S; Harder, Ross J

2017-02-08

Imaging the dynamical response of materials following ultrafast excitation can reveal energy transduction mechanisms and their dissipation pathways, as well as material stability under conditions far from equilibrium. Such dynamical behavior is challenging to characterize, especially operando at nanoscopic spatiotemporal scales. In this letter, we use X-ray coherent diffractive imaging to show that ultrafast laser excitation of a ZnO nanocrystal induces a rich set of deformation dynamics including characteristic "hard" or inhomogeneous and "soft" or homogeneous modes at different time scales, corresponding respectively to the propagation of acoustic phonons and resonant oscillation of the crystal. By integrating the 3D nanocrystal structure obtained from the ultrafast X-ray measurements with a continuum thermo-electro-mechanical finite element model, we elucidate the deformation mechanisms following laser excitation, in particular, a torsional mode that generates a 50% greater electric potential gradient than that resulting from the flexural mode. Understanding of the time-dependence of these mechanisms on ultrafast scales has significant implications for development of new materials for nanoscale power generation.

Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals

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

Cherukara, Mathew J.; Sasikumar, Kiran; Cha, Wonsuk

Imaging the dynamical response of materials following ultrafast excitation can reveal energy transduction mechanisms and their dissipation pathways, as well as material stability under conditions far from equilibrium. Such dynamical behaviour is challenging to characterize, especially operando at nanoscopic spatiotemporal scales. In this letter, we use x-ray coherent diffractive imaging to show that ultrafast laser excitation of a ZnO nanocrystal induces a rich set of deformation dynamics including characteristic ‘hard’ or inhomogeneous and ‘soft’ or homogeneous modes at different time scales, corresponding respectively to the propagation of acoustic phonons and resonant oscillation of the crystal. By integrating the 3D nanocrystalmore » structure obtained from the ultrafast x-ray measurements with a continuum thermo-electro-mechanical finite element model, we elucidate the deformation mechanisms following laser excitation, in particular, a torsional mode that generates a 50% greater electric potential gradient than that resulting from the flexural mode. Furthermore, understanding of the time-dependence of these mechanisms on ultrafast scales has significant implications for development of new materials for nanoscale power generation.« less

Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals

DOE PAGES

Cherukara, Mathew J.; Sasikumar, Kiran; Cha, Wonsuk; ...

2016-12-27

Imaging the dynamical response of materials following ultrafast excitation can reveal energy transduction mechanisms and their dissipation pathways, as well as material stability under conditions far from equilibrium. Such dynamical behaviour is challenging to characterize, especially operando at nanoscopic spatiotemporal scales. In this letter, we use x-ray coherent diffractive imaging to show that ultrafast laser excitation of a ZnO nanocrystal induces a rich set of deformation dynamics including characteristic ‘hard’ or inhomogeneous and ‘soft’ or homogeneous modes at different time scales, corresponding respectively to the propagation of acoustic phonons and resonant oscillation of the crystal. By integrating the 3D nanocrystalmore » structure obtained from the ultrafast x-ray measurements with a continuum thermo-electro-mechanical finite element model, we elucidate the deformation mechanisms following laser excitation, in particular, a torsional mode that generates a 50% greater electric potential gradient than that resulting from the flexural mode. Furthermore, understanding of the time-dependence of these mechanisms on ultrafast scales has significant implications for development of new materials for nanoscale power generation.« less

Ultrafast Magnetization Manipulation Using Single Femtosecond Light and Hot-Electron Pulses.

PubMed

Xu, Yong; Deb, Marwan; Malinowski, Grégory; Hehn, Michel; Zhao, Weisheng; Mangin, Stéphane

2017-11-01

Current-induced magnetization manipulation is a key issue for spintronic applications. This manipulation must be fast, deterministic, and nondestructive in order to function in device applications. Therefore, single- electronic-pulse-driven deterministic switching of the magnetization on the picosecond timescale represents a major step toward future developments of ultrafast spintronic systems. Here, the ultrafast magnetization dynamics in engineered Gd x [FeCo] 1- x -based structures are studied to compare the effect of femtosecond laser and hot-electron pulses. It is demonstrated that a single femtosecond hot-electron pulse causes deterministic magnetization reversal in either Gd-rich and FeCo-rich alloys similarly to a femtosecond laser pulse. In addition, it is shown that the limiting factor of such manipulation for perpendicular magnetized films arises from the formation of a multidomain state due to dipolar interactions. By performing time-resolved measurements under various magnetic fields, it is demonstrated that the same magnetization dynamics are observed for both light and hot-electron excitation, and that the full magnetization reversal takes place within 40 ps. The efficiency of the ultrafast current-induced magnetization manipulation is enhanced due to the ballistic transport of hot electrons before reaching the GdFeCo magnetic layer. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Femtosecond laser pulse induced phase transition of Cr-doped Sb2Te1 films studied with a pump-probe system

NASA Astrophysics Data System (ADS)

Jiang, Minghui; Wang, Qing; Lei, Kai; Wang, Yang; Liu, Bo; Song, Zhitang

2016-10-01

The Femtosecond laser pulse induced phase transition dynamics of Cr-doped Sb2Te1 films was studied by real-time reflectivity measurements with a pump-probe system. It was found that crystallization of the as-deposited CrxSb2Te1 phase-change thin films exhibits a multi-stage process lasting for about 40ns.The time required for the multi-stage process seems to be not related to the contents of Cr element. The durations of the crystallization and amorphization processes are approximately the same. Doping Cr into Sb2Te1 thin film can improve its photo-thermal stability without obvious change in the crystallization rate. Optical images and image intensity cross sections are used to visualize the transformed regions. This work may provide further insight into the phase-change mechanism of CrxSb2Te1 under extra-non-equilibrium conditions and aid to develop new ultrafast phase-change memory materials.

Hysteresis, nucleation and growth phenomena in spin-crossover solids

NASA Astrophysics Data System (ADS)

Ridier, Karl; Molnár, Gábor; Salmon, Lionel; Nicolazzi, William; Bousseksou, Azzedine

2017-12-01

The observation and the study of first-order phase transitions in cooperative spin-crossover (SCO) solids exhibiting hysteresis behaviours are of particular interest and currently constitute a burgeoning area in the field of bistable molecular materials. The understanding and the control of the transition mechanisms (nucleation and growth processes) and their dynamics within the hysteresis region appear to be a general and appealing problem from a fundamental point of view and for technological applications as well. This review reports on the recent progresses and most important findings made on the spatiotemporal dynamics of the spin transition in SCO solids, particularly through the universal nucleation and growth process. Both thermally induced and light-induced spin transitions are discussed. We open up this review to the central question of the evolution of the transition mechanisms and dynamics in SCO nano-objects, which constitute promising systems to reach ultra-fast switching, and the experimental issues inherent to such studies at the micro- and nanometric scale.

Pump-probe imaging of laser-induced periodic surface structures after ultrafast irradiation of Si

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

Murphy, Ryan D.; Torralva, Ben; Adams, David P.

2013-09-30

Ultrafast pump-probe microscopy has been used to investigate laser-induced periodic surface structure (LIPSS) formation on polished Si surfaces. A crater forms on the surface after irradiation by a 150 fs laser pulse, and a second, subsequent pulse forms LIPSS within the crater. Sequentially delayed images show that LIPSS with a periodicity slightly less than the fundamental laser wavelength of 780 nm appear on Si surfaces ∼50 ps after arrival of the second pump laser pulse, well after the onset of melting. LIPSS are observed on the same timescale as material removal, suggesting that their formation involves material ejection.

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.

DURIP: A Confocal Imaging System for Ultra-Fast Three-Dimensional Transport Studies in Thermal Management Applications

DTIC Science & Technology

2011-12-01

Transport Phenomena and Thermal Management Applications,” Proceedings of the XXVIII UIT Heat Transfer Conference, Brescia, Italy, June 21-23, 2010...measurements in microscale systems. The integrated confocal microscope system is a critical component to obtain understanding of fluid- heat ...objective of this work was to develop a high speed three-dimensional (3D) confocal imaging system to study coupled fluidic and heat transport

Watching ultrafast responses of structure and magnetism in condensed matter with momentum-resolved probes

PubMed Central

Johnson, S. L.; Savoini, M.; Beaud, P.; Ingold, G.; Staub, U.; Carbone, F.; Castiglioni, L.; Hengsberger, M.; Osterwalder, J.

2017-01-01

We present a non-comprehensive review of some representative experimental studies in crystalline condensed matter systems where the effects of intense ultrashort light pulses are probed using x-ray diffraction and photoelectron spectroscopy. On an ultrafast (sub-picosecond) time scale, conventional concepts derived from the assumption of thermodynamic equilibrium must often be modified in order to adequately describe the time-dependent changes in material properties. There are several commonly adopted approaches to this modification, appropriate in different experimental circumstances. One approach is to treat the material as a collection of quasi-thermal subsystems in thermal contact with each other in the so-called “N-temperature” models. On the other extreme, one can also treat the time-dependent changes as fully coherent dynamics of a sometimes complex network of excitations. Here, we present examples of experiments that fall into each of these categories, as well as experiments that partake of both models. We conclude with a discussion of the limitations and future potential of these concepts. PMID:29308418

Structural dynamics of lipid bilayers using ultrafast electron crystallography

NASA Astrophysics Data System (ADS)

Chen, Songye; Seidel, Marco; Zewail, Ahmed

2007-03-01

The structures and dynamics of bilayers of crystalline fatty acids and phospholipids were studied using ultrafast electron crystallography (UEC). The systems investigated are arachidic (eicosanoic) acid and dimyristoyl phosphatidic acid (DMPA), deposited on a substrate by the Langmuir-Blodgett technique. The atomic structures under different preparation conditions were determined. The structural dynamics following a temperature jump induced by femtosecond laser on the substrates were obtained and compared to the equilibrium temperature dependence.

Micro rectennas: Brownian ratchets for thermal-energy harvesting

NASA Astrophysics Data System (ADS)

Pan, Y.; Powell, C. V.; Song, A. M.; Balocco, C.

2014-12-01

We experimentally demonstrated the operation of a rectenna for harvesting thermal (blackbody) radiation and converting it into dc electric power. The device integrates an ultrafast rectifier, the self-switching nanodiode, with a wideband log-periodic spiral microantenna. The radiation from the thermal source drives the rectenna out of thermal equilibrium, permitting the rectification of the excess thermal fluctuations from the antenna. The power conversion efficiency increases with the source temperatures up to 0.02% at 973 K. The low efficiency is attributed mainly to the impedance mismatch between antenna and rectifier, and partially to the large field of view of the antenna. Our device not only opens a potential solution for harvesting thermal energy but also provides a platform for experimenting with Brownian ratchets.

RADIATION CHEMISTRY 2010 GORDON RESEARCH CONFERENCE JULY 18-23

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

Thomas Orlando

The 2010 Gordon Conference on Radiation Chemistry will present cutting edge research regarding the study of radiation-induced chemical transformations. Radiation Chemistry or 'high energy' chemistry is primarily initiated by ionizing radiation: i.e. photons or particles with energy sufficient to create conduction band electrons and 'holes', excitons, ionic and neutral free radicals, highly excited states, and solvated electrons. These transients often interact or 'react' to form products vastly different than those produced under thermal equilibrium conditions. The non-equilibrium, non-thermal conditions driving radiation chemistry exist in plasmas, star-forming regions, the outer solar system, nuclear reactors, nuclear waste repositories, radiation-based medical/clinical treatment centersmore » and in radiation/materials processing facilities. The 2010 conference has a strong interdisciplinary flavor with focus areas spanning (1) the fundamental physics and chemistry involved in ultrafast (atto/femtosecond) energy deposition events, (2) radiation-induced processes in biology (particularly spatially resolved studies), (3) radiation-induced modification of materials at the nanoscale and cosmic ray/x-ray mediated processes in planetary science/astrochemistry. While the conference concentrates on fundamental science, topical applied areas covered will also include nuclear power, materials/polymer processing, and clinical/radiation treatment in medicine. The Conference will bring together investigators at the forefront of their field, and will provide opportunities for junior scientists and graduate students to present work in poster format or as contributors to the Young Investigator session. The program and format provides excellent avenues to promote cross-disciplinary collaborations.« less

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.

Ultrafast surface carrier dynamics in the topological insulator Bi₂Te₃.

PubMed

Hajlaoui, M; Papalazarou, E; Mauchain, J; Lantz, G; Moisan, N; Boschetto, D; Jiang, Z; Miotkowski, I; Chen, Y P; Taleb-Ibrahimi, A; Perfetti, L; Marsi, M

2012-07-11

We discuss the ultrafast evolution of the surface electronic structure of the topological insulator Bi(2)Te(3) following a femtosecond laser excitation. Using time and angle-resolved photoelectron spectroscopy, we provide a direct real-time visualization of the transient carrier population of both the surface states and the bulk conduction band. We find that the thermalization of the surface states is initially determined by interband scattering from the bulk conduction band, lasting for about 0.5 ps; subsequently, few picoseconds are necessary for the Dirac cone nonequilibrium electrons to recover a Fermi-Dirac distribution, while their relaxation extends over more than 10 ps. The surface sensitivity of our measurements makes it possible to estimate the range of the bulk-surface interband scattering channel, indicating that the process is effective over a distance of 5 nm or less. This establishes a correlation between the nanoscale thickness of the bulk charge reservoir and the evolution of the ultrafast carrier dynamics in the surface Dirac cone.

Enhanced generation and anisotropic Coulomb scattering of hot electrons in an ultra-broadband plasmonic nanopatch metasurface

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

Sykes, Matthew E.; Stewart, Jon W.; Akselrod, Gleb M.

The creation of energetic electrons through plasmon excitation of nanostructures before thermalization has been proposed for a wide number of applications in optical energy conversion and ultrafast nanophotonics. However, the use of "nonthermal" electrons is primarily limited by both a low generation efficiency and their ultrafast decay. We report experimental and theoretical results on the use of broadband plasmonic nanopatch metasurfaces comprising a gold substrate coupled to silver nanocubes that produce large concentrations of hot electrons, which we measure using transient absorption spectroscopy. We find evidence for three subpopulations of nonthermal carriers which we propose arise from anisotropic electron-electron scatteringmore » within sp-bands near the Fermi surface. The bimetallic character of the metasurface strongly impacts the physics, with dissipation occurring primarily in the gold whereas the quantum process of hot electron generation takes place in both components. As a result, our calculations show that the choice of geometry and materials is crucial for producing strong ultrafast nonthermal electron components.« less

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.

Enhanced generation and anisotropic Coulomb scattering of hot electrons in an ultra-broadband plasmonic nanopatch metasurface

DOE PAGES

Sykes, Matthew E.; Stewart, Jon W.; Akselrod, Gleb M.; ...

2017-10-17

The creation of energetic electrons through plasmon excitation of nanostructures before thermalization has been proposed for a wide number of applications in optical energy conversion and ultrafast nanophotonics. However, the use of "nonthermal" electrons is primarily limited by both a low generation efficiency and their ultrafast decay. We report experimental and theoretical results on the use of broadband plasmonic nanopatch metasurfaces comprising a gold substrate coupled to silver nanocubes that produce large concentrations of hot electrons, which we measure using transient absorption spectroscopy. We find evidence for three subpopulations of nonthermal carriers which we propose arise from anisotropic electron-electron scatteringmore » within sp-bands near the Fermi surface. The bimetallic character of the metasurface strongly impacts the physics, with dissipation occurring primarily in the gold whereas the quantum process of hot electron generation takes place in both components. As a result, our calculations show that the choice of geometry and materials is crucial for producing strong ultrafast nonthermal electron components.« less

ENVIRONMENTAL APPLICATIONS OF THERMAL EXTRACTION CONE PENETROMETRY AND ULTRAFAST GAS CHROMATOGRAPHY/MASS SPECTROMETRY. (R826184)

EPA Science Inventory

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

Phonon-induced ultrafast band gap control in LaTiO3

NASA Astrophysics Data System (ADS)

Gu, Mingqiang; Rondinelli, James M.

We propose a route for ultrafast band gap engineering in correlated transition metal oxides by using optically driven phonons. We show that the ∖Gamma-point electron band energies can be deterministically tuned in the nonequilibrium state. Taking the Mott insulator LaTiO3 as an example, we show that such phonon-assisted processes dynamically induce an indirect-to-direct band gap transition or even a metal-to-insulator transition, depending on the electron correlation strength. We explain the origin of the dynamical band structure control and also establish its generality by examining related oxides. Lastly, we describe experimental routes to realize the band structure control with impulsive stimulated Raman scattering.

Dissipative rogue waves induced by soliton explosions in an ultrafast fiber laser.

PubMed

Liu, Meng; Luo, Ai-Ping; Xu, Wen-Cheng; Luo, Zhi-Chao

2016-09-01

We reported on the observation of dissipative rogue waves (DRWs) induced by soliton explosions in an ultrafast fiber laser. It was found that the soliton explosions could be obtained in the fiber laser at a critical pump power level. During the process of the soliton explosion, the high-amplitude waves that fulfill the rogue wave criteria could be detected. The appearance of the DRWs was identified by characterizing the intensity statistics of the time-stretched soliton profile based on the dispersive Fourier-transform method. Our findings provide the first experimental demonstration that the DRWs could be observed in the soliton explosion regime and further enhance the understanding of the physical mechanism of optical RW generation.

Periodic surface structure bifurcation induced by ultrafast laser generated point defect diffusion in GaAs

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

Abere, Michael J.; Yalisove, Steven M.; Torralva, Ben

2016-04-11

The formation of high spatial frequency laser induced periodic surface structures (HSFL) with period <0.3 λ in GaAs after irradiation with femtosecond laser pulses in air is studied. We have identified a point defect generation mechanism that operates in a specific range of fluences in semiconductors between the band-gap closure and ultrafast-melt thresholds that produces vacancy/interstitial pairs. Stress relaxation, via diffusing defects, forms the 350–400 nm tall and ∼90 nm wide structures through a bifurcation process of lower spatial frequency surface structures. The resulting HSFL are predominately epitaxial single crystals and retain the original GaAs stoichiometry.

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.

Laser-Induced Translative Hydrodynamic Mass Snapshots: Noninvasive Characterization and Predictive Modeling via Mapping at Nanoscale

NASA Astrophysics Data System (ADS)

Wang, X. W.; Kuchmizhak, A. A.; Li, X.; Juodkazis, S.; Vitrik, O. B.; Kulchin, Yu. N.; Zhakhovsky, V. V.; Danilov, P. A.; Ionin, A. A.; Kudryashov, S. I.; Rudenko, A. A.; Inogamov, N. A.

2017-10-01

Subwavelength structures (meta-atoms) with artificially engineered permittivity and permeability have shown promising applications for guiding and controlling the flow of electromagnetic energy on the nanoscale. Ultrafast laser nanoprinting emerges as a promising single-step, green and flexible technology in fabricating large-area arrays of meta-atoms through the translative or ablative modification of noble-metal thin films. Ultrafast laser energy deposition in noble-metal films produces irreversible, intricate nanoscale translative mass redistributions after resolidification of the transient thermally assisted hydrodynamic melt perturbations. Such mass redistribution results in the formation of a radially symmetric frozen surface with modified hidden nanofeatures, which strongly affect the optical response harnessed in plasmonic sensing and nonlinear optical applications. Here, we demonstrate that side-view electron microscopy and ion-beam cross sections together with low-energy electron x-ray dispersion microscopy provide exact information about such three-dimensional patterns, enabling an accurate acquisition of their cross-sectional mass distributions. Such nanoscale solidified structures are theoretically modeled, considering the underlying physical processes associated with laser-induced energy absorption, electron-ion energy exchange, acoustic relaxation, and hydrodynamic flows. A theoretical approach, separating slow and fast physical processes and combining hybrid analytical two-temperature calculations, scalable molecular-dynamics simulations, and a semianalytical thin-shell model is synergistically applied. These advanced characterization approaches are required for a detailed modeling of near-field electromagnetic response and pave the way to a fully automated noninvasive in-line control of a high-throughput and large-scale laser fabrication. This theoretical modeling provides an accurate prediction of scales and topographies of the laser-fabricated meta-atoms and metasurfaces.

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.

An ultrafast nanotip electron gun triggered by grating-coupled surface plasmons

NASA Astrophysics Data System (ADS)

Schröder, Benjamin; Sivis, Murat; Bormann, Reiner; Schäfer, Sascha; Ropers, Claus

2015-12-01

We demonstrate multiphoton photoelectron emission from gold nanotips induced by nanofocusing surface plasmons, resonantly excited on the tip shaft by a grating coupler. The tip is integrated into an electron gun assembly, which facilitates control over the spatial emission sites and allows us to disentangle direct grating emission from plasmon-triggered apex emission. The nanoscale source size of this electron gun concept enables highly coherent electron pulses with applications in ultrafast electron imaging and diffraction.

An ultrafast nanotip electron gun triggered by grating-coupled surface plasmons

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

Schröder, Benjamin; Sivis, Murat; Bormann, Reiner

We demonstrate multiphoton photoelectron emission from gold nanotips induced by nanofocusing surface plasmons, resonantly excited on the tip shaft by a grating coupler. The tip is integrated into an electron gun assembly, which facilitates control over the spatial emission sites and allows us to disentangle direct grating emission from plasmon-triggered apex emission. The nanoscale source size of this electron gun concept enables highly coherent electron pulses with applications in ultrafast electron imaging and diffraction.

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.

IR-Driven Ultrafast Transfer of Plasmonic Hot Electrons in Nonmetallic Branched Heterostructures for Enhanced H2 Generation.

PubMed

Zhang, Zhenyi; Jiang, Xiaoyi; Liu, Benkang; Guo, Lijiao; Lu, Na; Wang, Li; Huang, Jindou; Liu, Kuichao; Dong, Bin

2018-03-01

The ultrafast transfer of plasmon-induced hot electrons is considered an effective kinetics process to enhance the photoconversion efficiencies of semiconductors through strong localized surface plasmon resonance (LSPR) of plasmonic nanostructures. Although this classical sensitization approach is widely used in noble-metal-semiconductor systems, it remains unclear in nonmetallic plasmonic heterostructures. Here, by combining ultrafast transient absorption spectroscopy with theoretical simulations, IR-driven transfer of plasmon-induced hot electron in a nonmetallic branched heterostructure is demonstrated, which is fabricated through solvothermal growth of plasmonic W 18 O 49 nanowires (as branches) onto TiO 2 electrospun nanofibers (as backbones). The ultrafast transfer of hot electron from the W 18 O 49 branches to the TiO 2 backbones occurs within a timeframe on the order of 200 fs with very large rate constants ranging from 3.8 × 10 12 to 5.5 × 10 12 s -1 . Upon LSPR excitation by low-energy IR photons, the W 18 O 49 /TiO 2 branched heterostructure exhibits obviously enhanced catalytic H 2 generation from ammonia borane compared with that of W 18 O 49 nanowires. Further investigations by finely controlling experimental conditions unambiguously confirm that this plasmon-enhanced catalytic activity arises from the transfer of hot electron rather than from the photothermal effect. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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 terahertz control of extreme tunnel currents through single atoms on a silicon surface

NASA Astrophysics Data System (ADS)

Jelic, Vedran; Iwaszczuk, Krzysztof; Nguyen, Peter H.; Rathje, Christopher; Hornig, Graham J.; Sharum, Haille M.; Hoffman, James R.; Freeman, Mark R.; Hegmann, Frank A.

2017-06-01

Ultrafast control of current on the atomic scale is essential for future innovations in nanoelectronics. Extremely localized transient electric fields on the nanoscale can be achieved by coupling picosecond duration terahertz pulses to metallic nanostructures. Here, we demonstrate terahertz scanning tunnelling microscopy (THz-STM) in ultrahigh vacuum as a new platform for exploring ultrafast non-equilibrium tunnelling dynamics with atomic precision. Extreme terahertz-pulse-driven tunnel currents up to 107 times larger than steady-state currents in conventional STM are used to image individual atoms on a silicon surface with 0.3 nm spatial resolution. At terahertz frequencies, the metallic-like Si(111)-(7 × 7) surface is unable to screen the electric field from the bulk, resulting in a terahertz tunnel conductance that is fundamentally different than that of the steady state. Ultrafast terahertz-induced band bending and non-equilibrium charging of surface states opens new conduction pathways to the bulk, enabling extreme transient tunnel currents to flow between the tip and sample.

Ultrafast Electric Field Pulse Control of Giant Temperature Change in Ferroelectrics

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

Qi, Y.; Liu, S.; Lindenberg, A. M.

There is a surge of interest in developing environmentally friendly solid-state-based cooling technology. Here, we point out that a fast cooling rate (≈ 10 11 K/s) can be achieved by driving solid crystals to a high-temperature phase with a properly designed electric field pulse. Specifically, we predict that an ultrafast electric field pulse can cause a giant temperature decrease up to 32 K in PbTiO 3 occurring on few picosecond time scales. Here, we explain the underlying physics of this giant electric field pulse-induced temperature change with the concept of internal energy redistribution: the electric field does work on amore » ferroelectric crystal and redistributes its internal energy, and the way the kinetic energy is redistributed determines the temperature change and strongly depends on the electric field temporal profile. This concept is supported by our all-atom molecular dynamics simulations of PbTiO 3 and BaTiO 3. Moreover, this internal energy redistribution concept can also be applied to understand electrocaloric effect. We further propose new strategies for inducing giant cooling effect with ultrafast electric field pulse. This Letter offers a general framework to understand electric-field-induced temperature change and highlights the opportunities of electric field engineering for controlled design of fast and efficient cooling technology.« less

Ultrafast Electric Field Pulse Control of Giant Temperature Change in Ferroelectrics

DOE PAGES

Qi, Y.; Liu, S.; Lindenberg, A. M.; ...

2018-01-30

There is a surge of interest in developing environmentally friendly solid-state-based cooling technology. Here, we point out that a fast cooling rate (≈ 10 11 K/s) can be achieved by driving solid crystals to a high-temperature phase with a properly designed electric field pulse. Specifically, we predict that an ultrafast electric field pulse can cause a giant temperature decrease up to 32 K in PbTiO 3 occurring on few picosecond time scales. Here, we explain the underlying physics of this giant electric field pulse-induced temperature change with the concept of internal energy redistribution: the electric field does work on amore » ferroelectric crystal and redistributes its internal energy, and the way the kinetic energy is redistributed determines the temperature change and strongly depends on the electric field temporal profile. This concept is supported by our all-atom molecular dynamics simulations of PbTiO 3 and BaTiO 3. Moreover, this internal energy redistribution concept can also be applied to understand electrocaloric effect. We further propose new strategies for inducing giant cooling effect with ultrafast electric field pulse. This Letter offers a general framework to understand electric-field-induced temperature change and highlights the opportunities of electric field engineering for controlled design of fast and efficient cooling technology.« less

Ultrafast Electric Field Pulse Control of Giant Temperature Change in Ferroelectrics

NASA Astrophysics Data System (ADS)

Qi, Y.; Liu, S.; Lindenberg, A. M.; Rappe, A. M.

2018-01-01

There is a surge of interest in developing environmentally friendly solid-state-based cooling technology. Here, we point out that a fast cooling rate (≈1011 K /s ) can be achieved by driving solid crystals to a high-temperature phase with a properly designed electric field pulse. Specifically, we predict that an ultrafast electric field pulse can cause a giant temperature decrease up to 32 K in PbTiO3 occurring on few picosecond time scales. We explain the underlying physics of this giant electric field pulse-induced temperature change with the concept of internal energy redistribution: the electric field does work on a ferroelectric crystal and redistributes its internal energy, and the way the kinetic energy is redistributed determines the temperature change and strongly depends on the electric field temporal profile. This concept is supported by our all-atom molecular dynamics simulations of PbTiO3 and BaTiO3 . Moreover, this internal energy redistribution concept can also be applied to understand electrocaloric effect. We further propose new strategies for inducing giant cooling effect with ultrafast electric field pulse. This Letter offers a general framework to understand electric-field-induced temperature change and highlights the opportunities of electric field engineering for controlled design of fast and efficient cooling technology.

Investigation of the efficacy of ultrafast laser in large bowel excision

NASA Astrophysics Data System (ADS)

Mohanan, Syam Mohan P. C.; Beck, Rainer J.; Góra, Wojciech S.; Perry, Sarah L.; Shires, Mike; Jayne, David; Hand, Duncan P.; Shephard, Jonathan D.

2017-02-01

Local resection of early stage tumors in the large bowel via colonoscopy has been a widely accepted surgical modality for colon neoplasm treatment. The conventional electrocautery techniques used for the resection of neoplasia in the mucosal or submucosal layer of colon tissue has been shown to create obvious thermal necrosis to adjacent healthy tissues and lacks accuracy in resection. Ultrafast picosecond (ps) laser ablation using a wavelength of 1030 or 515 nm is a promising surgical tool to overcome the limitations seen with conventional surgical techniques. The purpose of this initial study is to analyze the depth of ablation or the extent of coagulation deployed by the laser as a function of pulse energy and fluence in an ex-vivo porcine model. Precise control of the depth of tissue removal is of paramount importance for bowel surgery where bowel perforation can lead to morbidity or mortality. Thus we investigate the regimes that are optimal for tissue resection and coagulation through plasma mediated ablation of healthy colon tissue. The ablated tissue samples were analyzed by standard histologic methods and a three dimensional optical profilometer technique. We demonstrate that ultrafast laser resection of colonic tissue can minimize the region of collateral thermal damage (<50 μm) with a controlled ablation depth. This surgical modality allows potentially easier removal of early stage lesions and has the capability to provide more control to the surgeon in comparison with a mechanical or electrocautery device.

Ultra-fast movies of thin-film laser ablation

NASA Astrophysics Data System (ADS)

Domke, Matthias; Rapp, Stephan; Schmidt, Michael; Huber, Heinz P.

2012-11-01

Ultra-short-pulse laser irradiation of thin molybdenum films from the glass substrate side initiates an intact Mo disk lift off free from thermal effects. For the investigation of the underlying physical effects, ultra-fast pump-probe microscopy is used to produce stop-motion movies of the single-pulse ablation process, initiated by a 660-fs laser pulse. The ultra-fast dynamics in the femtosecond and picosecond ranges are captured by stroboscopic illumination of the sample with an optically delayed probe pulse of 510-fs duration. The nanosecond and microsecond delay ranges of the probe pulse are covered by an electronically triggered 600-ps laser. Thus, the setup enables an observation of general laser ablation processes from the femtosecond delay range up to the final state. A comparison of time- and space-resolved observations of film and glass substrate side irradiation of a 470-nm molybdenum layer reveals the driving mechanisms of the Mo disk lift off initiated by glass-side irradiation. Observations suggest that a phase explosion generates a liquid-gas mixture in the molybdenum/glass interface about 10 ps after the impact of the pump laser pulse. Then, a shock wave and gas expansion cause the molybdenum layer to bulge, while the enclosed liquid-gas mixture cools and condenses at delay times in the 100-ps range. The bulging continues for approximately 20 ns, when an intact Mo disk shears and lifts off at a velocity of above 70 m/s. As a result, the remaining hole is free from thermal effects.

Towards validated chemistry at extreme conditions: reactive MD simulations of shocked Polyvinyl Nitrate and Nitromethane

NASA Astrophysics Data System (ADS)

Islam, Md Mahbubul; Strachan, Alejandro

A detailed atomistic-level understanding of the ultrafast chemistry of detonation processes of high energy materials is crucial to understand their performance and safety. Recent advances in laser shocks and ultra-fast spectroscopy is yielding the first direct experimental evidence of chemistry at extreme conditions. At the same time, reactive molecular dynamics (MD) in current high-performance computing platforms enable an atomic description of shock-induced chemistry with length and timescales approaching those of experiments. We use MD simulations with the reactive force field ReaxFF to investigate the shock-induced chemical decomposition mechanisms of polyvinyl nitrate (PVN) and nitromethane (NM). The effect of shock pressure on chemical reaction mechanisms and kinetics of both the materials are investigated. For direct comparison of our simulation results with experimentally derived IR absorption data, we performed spectral analysis using atomistic velocity at various shock conditions. The combination of reactive MD simulations and ultrafast spectroscopy enables both the validation of ReaxFF at extreme conditions and contributes to the interpretation of the experimental data relating changes in spectral features to atomic processes. Office of Naval Research MURI program.

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

Femtosecond pulsed laser processing of electronic materials: Fundamentals and micro/nano-scale applications

NASA Astrophysics Data System (ADS)

Choi, Tae-Youl

Ultra-short pulsed laser radiation has been shown to be effective for precision materials processing and surface micro-modification. One of advantages is the substantial reduction of the heat penetration depth, which leads to minimal lateral damage. Other advantages include non-thermal nature of ablation process, controlled ablation and ideal characteristics for precision micro-structuring. Yet, fundamental questions remain unsolved regarding the nature of melting and ablation mechanisms in femtosecond laser processing of materials. In addition to micro engineering problems, nano-structuring and nano-fabrication are emerging fields that are of particular interest in conjunction with femtosecond laser processing. A comprehensive experimental study as well as theoretical development is presented to address these issues. Ultra-short pulsed laser irradiation was used to crystallize 100 nm amorphous silicon (a-Si) films. The crystallization process was observed by time-resolved pump-and-probe reflection imaging in the range of 0.2 ps to 100 ns. The in-situ images in conjunction with post-processed SEM and AFM mapping of the crystallized structure provide evidence for non-thermal ultra-fast phase transition and subsequent surface-initiated crystallization. Mechanisms of ultra-fast laser-induced ablation on crystalline silicon and copper are investigated by time-resolved pump-and-probe microscopy in normal imaging and shadowgraph arrangements. A one-dimensional model of the energy transport is utilized to predict the carrier temperature and lattice temperature as well as the electron and vapor flux emitted from the surface. The temporal delay between the pump and probe pulses was set by a precision translation stage up to about 500 ps and then extended to the nanosecond regime by an optical fiber assembly. The ejection of material was observed at several picoseconds to tens of nanoseconds after the main (pump) pulse by high-resolution, ultra-fast shadowgraphs. The ultrashort laser pulse accompanied by the pre-pulse induces air breakdown that can be detrimental to materials processing. A time-resolved pump-and-probe experiment provides distinct evidence for the occurrence of an air plasma and air breakdown. This highly nonlinear phenomenon takes place before the commencement of the ablation process, which is traced beyond elapsed time of the order of 10 ps with respect to the ablating pulse. The nonlinear refractive index of the generated air plasma is calculated as a function of electron density. The self-focusing of the main pulse is identified by the third order nonlinear susceptibility. A crystalline silicon sample is subjected to two optically separated ultra-fast laser pulses of full-width-half-maximum (FWHM) duration of about 80 femtoseconds. These pulses are delivered at wavelength, lambda = 800 nm. Femtosecond-resolved imaging pump-and-probe experiments in reflective and Schlieren configurations have been performed to investigate plasma dynamics and shock wave propagation during the sample ablation process. By using a diffractive optical element (DOE) for beam shaping, microchannels were fabricated. A super-long working distance objective lens was used to machine silicon materials in the sub-micrometer scale. As an extension of micro-machining, the finite difference time domain (FDTD) method is used to assess the feasibility of using near-field distribution of laser light. Gold coated films were machined with nano-scale dimensions and characterized with atomic force microscopy (AFM).

Micro rectennas: Brownian ratchets for thermal-energy harvesting

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

Pan, Y.; Powell, C. V.; Balocco, C., E-mail: claudio.balocco@durham.ac.uk

2014-12-22

We experimentally demonstrated the operation of a rectenna for harvesting thermal (blackbody) radiation and converting it into dc electric power. The device integrates an ultrafast rectifier, the self-switching nanodiode, with a wideband log-periodic spiral microantenna. The radiation from the thermal source drives the rectenna out of thermal equilibrium, permitting the rectification of the excess thermal fluctuations from the antenna. The power conversion efficiency increases with the source temperatures up to 0.02% at 973 K. The low efficiency is attributed mainly to the impedance mismatch between antenna and rectifier, and partially to the large field of view of the antenna. Our devicemore » not only opens a potential solution for harvesting thermal energy but also provides a platform for experimenting with Brownian ratchets.« less

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.

The link between tissue elasticity and thermal dose in vivo

NASA Astrophysics Data System (ADS)

Sapin-de Brosses, Emilie; Pernot, Mathieu; Tanter, Mickaël

2011-12-01

The objective of this study was to investigate in vivo the relationship between stiffness and thermal dose. For this purpose, shear wave elastography (SWE)—a novel ultrasound-based technique for real-time mapping of the stiffness of biological soft tissues—is performed in temperature-controlled experiments. Experiments were conducted on nine anesthetized rats. Their right leg was put in a thermo-regulated waterbath. The right leg of each animal was heated at one particular temperature between 38 °C and 48.5 °C for 15 min to 3 h. Shear waves were generated in the muscle using the acoustic radiation force induced by a linear ultrasonic probe. The shear wave propagation was imaged in real time by the probe using an ultrafast scanner prototype (10 000 frames s-1). The local tissue stiffness was derived from the shear wave speed. Two optical fiber sensors were inserted into the muscle to measure in situ the temperature. Stiffness was found to increase strongly during the experiments. When expressed as a function of the thermal dose, the stiffness curves were found to be the same for all experiments. A thermal dose threshold was found at 202 min for an eightfold stiffness increase. Finally, the time-temperature relationship was established for different stiffness ratios. The slope of the time-temperature relationship based on stiffness measurements was found identical to the one obtained for cell death in the seminal paper on the thermal dose by Sapareto and Dewey in 1984 (Int. J. Radiat. Oncol. Biol. Phys. 10 787-800). The present results highlight the stiffness increase as a good indicator of thermal necrosis. SWE imaging can be used in vivo for necrosis threshold determination in thermal therapy.

Coherent helix vacancy phonon and its ultrafast dynamics waning in topological Dirac semimetal C d3A s2

NASA Astrophysics Data System (ADS)

Sun, Fei; Wu, Q.; Wu, Y. L.; Zhao, H.; Yi, C. J.; Tian, Y. C.; Liu, H. W.; Shi, Y. G.; Ding, H.; Dai, X.; Richard, P.; Zhao, Jimin

2017-06-01

We report an ultrafast lattice dynamics investigation of the topological Dirac semimetal C d3A s2 . A coherent phonon beating among three evenly spaced A1 g optical phonon modes (of frequencies 1.80, 1.96, and 2.11 THz, respectively) is unambiguously observed. The two side modes originate from the counter helixes composing Cd vacancies. Significantly, such helix vacancy-induced phonon (HVP) modes experience prominent extra waning in their ultrafast dynamics as temperature increases, which is immune to the central mode. Above 200 K, the HVP becomes inactive, which may potentially affect the topological properties. Our results in the lattice degree of freedom suggest the indispensable role of temperature in considering topological properties of such quantum materials.

Combined passive detection and ultrafast active imaging of cavitation events induced by short pulses of high-intensity ultrasound.

PubMed

Gateau, Jérôme; Aubry, Jean-François; Pernot, Mathieu; Fink, Mathias; Tanter, Mickaël

2011-03-01

The activation of natural gas nuclei to induce larger bubbles is possible using short ultrasonic excitations of high amplitude, and is required for ultrasound cavitation therapies. However, little is known about the distribution of nuclei in tissues. Therefore, the acoustic pressure level necessary to generate bubbles in a targeted zone and their exact location are currently difficult to predict. To monitor the initiation of cavitation activity, a novel all-ultrasound technique sensitive to single nucleation events is presented here. It is based on combined passive detection and ultrafast active imaging over a large volume using the same multi-element probe. Bubble nucleation was induced using a focused transducer (660 kHz, f-number = 1) driven by a high-power electric burst (up to 300 W) of one to two cycles. Detection was performed with a linear array (4 to 7 MHz) aligned with the single-element focal point. In vitro experiments in gelatin gel and muscular tissue are presented. The synchronized passive detection enabled radio-frequency data to be recorded, comprising high-frequency coherent wave fronts as signatures of the acoustic emissions linked to the activation of the nuclei. Active change detection images were obtained by subtracting echoes collected in the unnucleated medium. These indicated the appearance of stable cavitating regions. Because of the ultrafast frame rate, active detection occurred as quickly as 330 μs after the high-amplitude excitation and the dynamics of the induced regions were studied individually.

Combined passive detection and ultrafast active imaging of cavitation events induced by short pulses of high-intensity ultrasound

PubMed Central

Gateau, Jérôme; Aubry, Jean-François; Pernot, Mathieu; Fink, Mathias; Tanter, Mickaël

2011-01-01

The activation of natural gas nuclei to induce larger bubbles is possible using short ultrasonic excitations of high amplitude, and is required for ultrasound cavitation therapies. However, little is known about the distribution of nuclei in tissues. Therefore, the acoustic pressure level necessary to generate bubbles in a targeted zone and their exact location are currently difficult to predict. In order to monitor the initiation of cavitation activity, a novel all-ultrasound technique sensitive to single nucleation events is presented here. It is based on combined passive detection and ultrafast active imaging over a large volume and with the same multi-element probe. Bubble nucleation was induced with a focused transducer (660kHz, f#=1) driven by a high power (up to 300 W) electric burst of one to two cycles. Detection was performed with a linear array (4–7MHz) aligned with the single-element focal point. In vitro experiments in gelatin gel and muscular tissue are presented. The synchronized passive detection enabled radio-frequency data to be recorded, comprising high-frequency coherent wave fronts as signatures of the acoustic emissions linked to the activation of the nuclei. Active change detection images were obtained by subtracting echoes collected in the unucleated medium. These indicated the appearance of stable cavitating regions. Thanks to the ultrafast frame rate, active detection occurred as soon as 330 μs after the high amplitude excitation and the dynamics of the induced regions were studied individually. PMID:21429844

Ultrafast light-induced symmetry changes in single BaTiO 3 nanowires

DOE PAGES

Kuo, Yi -Hong; Nah, Sanghee; He, Kai; ...

2017-01-23

The coupling of light to nanoscale ferroelectric materials enables novel means of controlling their coupled degrees of freedom and engineering new functionality. Here we present femtosecond time-resolution nonlinear-optical measurements of light-induced dynamics within single ferroelectric barium titanate nanowires. By analyzing the time-dependent and polarization-dependent second harmonic intensity generated by the nanowire, we identify its crystallographic orientation and then make use of this information in order to probe its dynamic structural response and change in symmetry. Here, we show that photo-excitation leads to ultrafast, non-uniform modulations in the second order nonlinear susceptibility tensor, indicative of changes in the local symmetry ofmore » the nanostructure occurring on sub-picosecond time-scales.« less

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 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.

Electron-mediated relaxation following ultrafast pumping of strongly correlated materials: model evidence of a correlation-tuned crossover between thermal and nonthermal states.

PubMed

Moritz, B; Kemper, A F; Sentef, M; Devereaux, T P; Freericks, J K

2013-08-16

We examine electron-electron mediated relaxation following ultrafast electric field pump excitation of the fermionic degrees of freedom in the Falicov-Kimball model for correlated electrons. The results reveal a dichotomy in the temporal evolution of the system as one tunes through the Mott metal-to-insulator transition: in the metallic regime relaxation can be characterized by evolution toward a steady state well described by Fermi-Dirac statistics with an increased effective temperature; however, in the insulating regime this quasithermal paradigm breaks down with relaxation toward a nonthermal state with a complicated electronic distribution as a function of momentum. We characterize the behavior by studying changes in the energy, photoemission response, and electronic distribution as functions of time. This relaxation may be observable qualitatively on short enough time scales that the electrons behave like an isolated system not in contact with additional degrees of freedom which would act as a thermal bath, especially when using strong driving fields and studying materials whose physics may manifest the effects of correlations.

Optimal control of laser-induced spin-orbit mediated ultrafast demagnetization

NASA Astrophysics Data System (ADS)

Elliott, P.; Krieger, K.; Dewhurst, J. K.; Sharma, S.; Gross, E. K. U.

2016-01-01

Laser induced ultrafast demagnetization is the process whereby the magnetic moment of a ferromagnetic material is seen to drop significantly on a timescale of 10-100 s of femtoseconds due to the application of a strong laser pulse. If this phenomenon can be harnessed for future technology, it offers the possibility for devices operating at speeds several orders of magnitude faster than at present. A key component to successful transfer of such a process to technology is the controllability of the process, i.e. that it can be tuned in order to overcome the practical and physical limitations imposed on the system. In this paper, we demonstrate that the spin-orbit mediated form of ultrafast demagnetization recently investigated (Krieger et al 2015 J. Chem. Theory Comput. 11 4870) by ab initio time-dependent density functional theory (TDDFT) can be controlled. To do so we use quantum optimal control theory (OCT) to couple our TDDFT simulations to the optimization machinery of OCT. We show that a laser pulse can be found which maximizes the loss of moment within a given time interval while subject to several practical and physical constraints. Furthermore we also include a constraint on the fluence of the laser pulses and find the optimal pulse that combines significant demagnetization with a desire for less powerful pulses. These calculations demonstrate optimal control is possible for spin-orbit mediated ultrafast demagnetization and lays the foundation for future optimizations/simulations which can incorporate even more constraints.

From Computational Photobiology to the Design of Vibrationally Coherent Molecular Devices and Motors

NASA Astrophysics Data System (ADS)

Olivucci, Massimo

2014-03-01

In the past multi-configurational quantum chemical computations coupled with molecular mechanics force fields have been employed to investigate spectroscopic, thermal and photochemical properties of visual pigments. Here we show how the same computational technology can nowadays be used to design, characterize and ultimately, prepare light-driven molecular switches which mimics the photophysics of the visual pigment bovine rhodopsin (Rh). When embedded in the protein cavity the chromophore of Rh undergoes an ultrafast and coherent photoisomerization. In order to design a synthetic chromophore displaying similar properties in common solvents, we recently focused on indanylidene-pyrroline (NAIP) systems. We found that these systems display light-induced ground state coherent vibrational motion similar to the one detected in Rh. Semi-classical trajectories provide a mechanistic description of the structural changes associated to the observed coherent motion which is shown to be ultimately due to periodic changes in the π-conjugation.

Ultrafast exciton migration in an HJ-aggregate: Potential surfaces and quantum dynamics

NASA Astrophysics Data System (ADS)

Binder, Robert; Polkehn, Matthias; Ma, Tianji; Burghardt, Irene

2017-01-01

Quantum dynamical and electronic structure calculations are combined to investigate the mechanism of exciton migration in an oligothiophene HJ aggregate, i.e., a combination of oligomer chains (J-type aggregates) and stacked aggregates of such chains (H-type aggregates). To this end, a Frenkel exciton model is parametrized by a recently introduced procedure [Binder et al., J. Chem. Phys. 141, 014101 (2014)] which uses oligomer excited-state calculations to perform an exact, point-wise mapping of coupled potential energy surfaces to an effective Frenkel model. Based upon this parametrization, the Multi-Layer Multi-Configuration Time-Dependent Hartree (ML-MCTDH) method is employed to investigate ultrafast dynamics of exciton transfer in a small, asymmetric HJ aggregate model composed of 30 sites and 30 active modes. For a partially delocalized initial condition, it is shown that a torsional defect confines the trapped initial exciton, and planarization induces an ultrafast resonant transition between an HJ-aggregated segment and a covalently bound "dangling chain" end. This model is a minimal realization of experimentally investigated mixed systems exhibiting ultrafast exciton transfer between aggregated, highly planarized chains and neighboring disordered segments.

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 shock-induced orientation of polycrystalline films: Applications to high explosives

NASA Astrophysics Data System (ADS)

Franken, Jens; Hambir, Selezion A.; Dlott, Dana D.

1999-02-01

Tiny laser-driven shock waves of ˜5 GPa pressure (nanoshocks) are used to study fast mechanical processes occurring in a thin layer of polycrystalline insensitive energetic material, (3-nitro-1,2,4-triazol-5-one) (NTO). Ultrafast coherent Raman spectroscopy of shocked NTO shows the existence of three distinct mechanical processes. Very fast (˜600 ps) changes in intensity and the appearance of new transitions are associated with the uniaxial nature of compression by the shock front. Frequency shifting and broadening processes which track the ˜2 ns duration nanoshock are associated with transient changes in density and temperature. A novel slower process (5-10 ns) starts as the shock begins to unload, and continues for several nanoseconds after the shock is over, resulting in changes of widths and intensities of several vibrational transitions. By comparing ultrafast spectra to static Raman spectra of single NTO crystals in various orientations, it is concluded that this process involves shock-induced partial orientation of the crystals in the NTO layer. The NTO crystals are oriented faster than the time scale for initiating chemical reactions. The sensitivity of explosive crystals to shock initiation may depend dramatically on the orientation of the crystal relative to the direction of shock propagation, so the implications of fast shock-induced orientation for energetic materials initiation are discussed briefly.

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.

Following strain-induced mosaicity changes of ferroelectric thin films by ultrafast reciprocal space mapping.

PubMed

Schick, D; Bojahr, A; Herzog, M; Gaal, P; Vrejoiu, I; Bargheer, M

2013-03-01

We investigate coherent phonon propagation in a thin film of ferroelectric PbZr(0.2)Ti(0.8)O(3) (PZT) by ultrafast x-ray diffraction experiments, which are analyzed as time-resolved reciprocal space mapping in order to observe the in- and out-of-plane structural dynamics, simultaneously. The mosaic structure of the PZT leads to a coupling of the excited out-of-plane expansion to in-plane lattice dynamics on a picosecond time scale, which is not observed for out-of-plane compression.

Ultrafast magnetic vortex core switching driven by the topological inverse Faraday effect.

PubMed

Taguchi, Katsuhisa; Ohe, Jun-ichiro; Tatara, Gen

2012-09-21

We present a theoretical discovery of an unconventional mechanism of inverse Faraday effect which acts selectively on topological magnetic structures. The effect, topological inverse Faraday effect, is induced by the spin Berry's phase of the magnetic structure when a circularly polarized light is applied. Thus a spin-orbit interaction is not necessary unlike that in the conventional inverse Faraday effect. We demonstrate by numerical simulation that topological inverse Faraday effect realizes ultrafast switching of a magnetic vortex within a switching time of 150 ps without magnetic field.

Femtosecond measurements of near-infrared pulse induced mid-infrared transmission modulation of quantum cascade lasers

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

Cai, Hong; Liu, Sheng; Center for Advanced Studied in Photonics Research

2014-05-26

We temporally resolved the ultrafast mid-infrared transmission modulation of quantum cascade lasers (QCLs) using a near-infrared pump/mid-infrared probe technique at room temperature. Two different femtosecond wavelength pumps were used with photon energy above and below the quantum well (QW) bandgap. The shorter wavelength pump modulates the mid-infrared probe transmission through interband transition assisted mechanisms, resulting in a high transmission modulation depth and several nanoseconds recovery lifetime. In contrast, pumping with a photon energy below the QW bandgap induces a smaller transmission modulation depth but much faster (several picoseconds) recovery lifetime, attributed to intersubband transition assisted mechanisms. The latter ultrafast modulationmore » (>60 GHz) could provide a potential way to realize fast QCL based free space optical communication.« less

Ultra-fast electron capture by electrosterically-stabilized gold nanoparticles.

PubMed

Ghandi, Khashayar; Findlater, Alexander D; Mahimwalla, Zahid; MacNeil, Connor S; Awoonor-Williams, Ernest; Zahariev, Federico; Gordon, Mark S

2015-07-21

Ultra-fast pre-solvated electron capture has been observed for aqueous solutions of room-temperature ionic liquid (RTIL) surface-stabilized gold nanoparticles (AuNPs; ∼9 nm). The extraordinarily large inverse temperature dependent rate constants (k(e)∼ 5 × 10(14) M(-1) s(-1)) measured for the capture of electrons in solution suggest electron capture by the AuNP surface that is on the timescale of, and therefore in competition with, electron solvation and electron-cation recombination reactions. The observed electron transfer rates challenge the conventional notion that radiation induced biological damage would be enhanced in the presence of AuNPs. On the contrary, AuNPs stabilized by non-covalently bonded ligands demonstrate the potential to quench radiation-induced electrons, indicating potential applications in fields ranging from radiation therapy to heterogeneous catalysis.

Confocal Raman imaging of optical waveguides in LiNbO3 fabricated by ultrafast high-repetition rate laser-writing.

PubMed

Ródenas, Airán; Nejadmalayeri, Amir H; Jaque, Daniel; Herman, Peter

2008-09-01

We report on the confocal Raman characterization of the micro-structural lattice changes induced during the high-repetition rate ultrafast laser writing of buried optical waveguides in lithium niobate (LiNbO(3)) crystals. While the laser beam focal volume is characterized by a significant lattice expansion together with a high defect concentration, the adjacent waveguide zone is largely free of defects, undergoing only slight rearrangement of the oxygen octahedron in the LiNbO(3) lattice. The close proximity of these two zones has been found responsible for the propagation losses of the guided light. Subjacent laser-induced periodic micro-structures have been also observed inside the laser focal volume, and identified with a strong periodic distribution of lattice defects.

Modulation of ultrafast laser-induced magnetization precession in BiFeO3-coated La0.67Sr0.33MnO3 thin films

NASA Astrophysics Data System (ADS)

Wan, Qian; Jin, KuiJuan; Wang, JieSu; Yao, HongBao; Gu, JunXing; Guo, HaiZhong; Xu, XiuLai; Yang, GuoZhen

2017-04-01

The ultrafast laser-excited magnetization dynamics of ferromagnetic (FM) La0.67Sr0.33MnO3 (LSMO) thin films with BiFeO3 (BFO) coating layers grown by laser molecular beam epitaxy are investigated using the optical pump-probe technique. Uniform magnetization precessions are observed in the films under an applied external magnetic field by measuring the time-resolved magneto-optical Kerr effect. The magnetization precession frequencies of the LSMO thin films with the BFO coating layers are lower than those of uncoated LSMO films, which is attributed to the suppression of the anisotropy field induced by the exchange interaction at the interface between the antiferromagnetic order of BFO and the FM order of LSMO.

Vitreous Cryopreservation of Human Umbilical Vein Endothelial Cells with Low Concentration of Cryoprotective Agents for Vascular Tissue Engineering

PubMed Central

Zheng, Yuanyuan; Panhwar, Fazil

2016-01-01

Cryopreservation of human umbilical vein endothelial cells (HUVECs) is important to tissue engineering applications and the study of the role of endothelial cells in cardiovascular and cerebrovascular diseases. The traditional methods for cryopreservation by vitrification (cooling samples to a cryogenic temperature without apparent freezing) using high concentration of cryoprotective agents (CPAs) and slow freezing are suboptimal due to the severe toxicity of high concentration of CPAs and ice formation-induced cryoinjuries, respectively. In this study, we developed a method to cryopreserve HUVECs by vitrification with low concentration of CPAs. This is achieved by optimizing the CPAs and using highly thermally conductive quartz capillary (QC) to contain samples for vitrification. The latter minimizes the thermal mass to create ultra-fast cooling/warming rates. Our data demonstrate that HUVECs can be vitrified in the QC using 1.4 mol/L ethylene glycol and 1.1 mol/L dimethyl sulfoxide with more than 90% viability. Moreover, this method significantly improves the attachment efficiency of the cryopreserved HUVECs. The attached cells post-cryopreservation proliferate similarly to fresh cells. Therefore, this study may provide an effective vitrification technique to bank HUVECs for vascular tissue engineering and other applications. PMID:27673413

Ultrafast Direct Modulation of a Single-Mode Photonic Crystal Nanocavity Light-Emitting Diode

DTIC Science & Technology

2011-11-15

nanocavity laser with world record low threshold of 208 nW based on a lateral p-i-n junction defined by ion implantation in gallium arsenide6. This...recombination effects are mini- mized. In contrast, at room temperature, thermal excitation of car- riers depopulates the quantum dots much quicker than does Pur

Ultrafast nonthermal heating of water initiated by an X-ray Free-Electron Laser.

PubMed

Beyerlein, Kenneth R; Jönsson, H Olof; Alonso-Mori, Roberto; Aquila, Andrew; Bajt, Saša; Barty, Anton; Bean, Richard; Koglin, Jason E; Messerschmidt, Marc; Ragazzon, Davide; Sokaras, Dimosthenis; Williams, Garth J; Hau-Riege, Stefan; Boutet, Sébastien; Chapman, Henry N; Tîmneanu, Nicuşor; Caleman, Carl

2018-05-29

The bright ultrafast pulses of X-ray Free-Electron Lasers allow investigation into the structure of matter under extreme conditions. We have used single pulses to ionize and probe water as it undergoes a phase transition from liquid to plasma. We report changes in the structure of liquid water on a femtosecond time scale when irradiated by single 6.86 keV X-ray pulses of more than 10 6 J/cm 2 These observations are supported by simulations based on molecular dynamics and plasma dynamics of a water system that is rapidly ionized and driven out of equilibrium. This exotic ionic and disordered state with the density of a liquid is suggested to be structurally different from a neutral thermally disordered state.

Watching proton transfer in real time: Ultrafast photoionization-induced proton transfer in phenol-ammonia complex cation.

PubMed

Shen, Ching-Chi; Tsai, Tsung-Ting; Wu, Jun-Yi; Ho, Jr-Wei; Chen, Yi-Wei; Cheng, Po-Yuan

2017-10-28

In this paper, we give a full account of our previous work [C. C. Shen et al., J. Chem. Phys. 141, 171103 (2014)] on the study of an ultrafast photoionization-induced proton transfer (PT) reaction in the phenol-ammonia (PhOH-NH 3 ) complex using ultrafast time-resolved ion photofragmentation spectroscopy implemented by the photoionization-photofragmentation pump-probe detection scheme. Neutral PhOH-NH 3 complexes prepared in a free jet are photoionized by femtosecond 1 + 1 resonance-enhanced multiphoton ionization via the S 1 state. The evolving cations are then probed by delayed pulses that result in ion fragmentation, and the ionic dynamics is followed by measuring the parent-ion depletion as a function of the pump-probe delay time. By comparing with systems in which PT is not feasible and the steady-state ion photofragmentation spectra, we concluded that the observed temporal evolutions of the transient ion photofragmentation spectra are consistent with an intracomplex PT reaction after photoionization from the initial non-PT to the final PT structures. Our experiments revealed that PT in [PhOH-NH 3 ] + cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ∼70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the time scale to complete the reaction can be much slower and is determined by the rate of energy dissipation into other modes.

Watching proton transfer in real time: Ultrafast photoionization-induced proton transfer in phenol-ammonia complex cation

NASA Astrophysics Data System (ADS)

Shen, Ching-Chi; Tsai, Tsung-Ting; Wu, Jun-Yi; Ho-Wei, Jr.; Chen, Yi-Wei; Cheng, Po-Yuan

2017-10-01

In this paper, we give a full account of our previous work [C. C. Shen et al., J. Chem. Phys. 141, 171103 (2014)] on the study of an ultrafast photoionization-induced proton transfer (PT) reaction in the phenol-ammonia (PhOH-NH3) complex using ultrafast time-resolved ion photofragmentation spectroscopy implemented by the photoionization-photofragmentation pump-probe detection scheme. Neutral PhOH-NH3 complexes prepared in a free jet are photoionized by femtosecond 1 + 1 resonance-enhanced multiphoton ionization via the S1 state. The evolving cations are then probed by delayed pulses that result in ion fragmentation, and the ionic dynamics is followed by measuring the parent-ion depletion as a function of the pump-probe delay time. By comparing with systems in which PT is not feasible and the steady-state ion photofragmentation spectra, we concluded that the observed temporal evolutions of the transient ion photofragmentation spectra are consistent with an intracomplex PT reaction after photoionization from the initial non-PT to the final PT structures. Our experiments revealed that PT in [PhOH-NH3]+ cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ˜70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the time scale to complete the reaction can be much slower and is determined by the rate of energy dissipation into other modes.

Spectral mapping of thermal conductivity through nanoscale ballistic transport

NASA Astrophysics Data System (ADS)

Hu, Yongjie; Zeng, Lingping; Minnich, Austin J.; Dresselhaus, Mildred S.; Chen, Gang

2015-08-01

Controlling thermal properties is central to many applications, such as thermoelectric energy conversion and the thermal management of integrated circuits. Progress has been made over the past decade by structuring materials at different length scales, but a clear relationship between structure size and thermal properties remains to be established. The main challenge comes from the unknown intrinsic spectral distribution of energy among heat carriers. Here, we experimentally measure this spectral distribution by probing quasi-ballistic transport near nanostructured heaters down to 30 nm using ultrafast optical spectroscopy. Our approach allows us to quantify up to 95% of the total spectral contribution to thermal conductivity from all phonon modes. The measurement agrees well with multiscale and first-principles-based simulations. We further demonstrate the direct construction of mean free path distributions. Our results provide a new fundamental understanding of thermal transport and will enable materials design in a rational way to achieve high performance.

Self-amplified photo-induced gap quenching in a correlated electron material

PubMed Central

Mathias, S.; Eich, S.; Urbancic, J.; Michael, S.; Carr, A. V.; Emmerich, S.; Stange, A.; Popmintchev, T.; Rohwer, T.; Wiesenmayer, M.; Ruffing, A.; Jakobs, S.; Hellmann, S.; Matyba, P.; Chen, C.; Kipp, L.; Bauer, M.; Kapteyn, H. C.; Schneider, H. C.; Rossnagel, K.; Murnane, M. M.; Aeschlimann, M.

2016-01-01

Capturing the dynamic electronic band structure of a correlated material presents a powerful capability for uncovering the complex couplings between the electronic and structural degrees of freedom. When combined with ultrafast laser excitation, new phases of matter can result, since far-from-equilibrium excited states are instantaneously populated. Here, we elucidate a general relation between ultrafast non-equilibrium electron dynamics and the size of the characteristic energy gap in a correlated electron material. We show that carrier multiplication via impact ionization can be one of the most important processes in a gapped material, and that the speed of carrier multiplication critically depends on the size of the energy gap. In the case of the charge-density wave material 1T-TiSe2, our data indicate that carrier multiplication and gap dynamics mutually amplify each other, which explains—on a microscopic level—the extremely fast response of this material to ultrafast optical excitation. PMID:27698341

Concerted electron-proton transfer in the optical excitation of hydrogen-bonded dyes

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

Westlake, Brittany C.; Brennaman, Kyle M.; Concepcion, Javier J.

2011-05-24

The simultaneous, concerted transfer of electrons and protons—electron-proton transfer (EPT)—is an important mechanism utilized in chemistry and biology to avoid high energy intermediates. There are many examples of thermally activated EPT in ground-state reactions and in excited states following photoexcitation and thermal relaxation. Here we report application of ultrafast excitation with absorption and Raman monitoring to detect a photochemically driven EPT process (photo-EPT). In this process, both electrons and protons are transferred during the absorption of a photon. Photo-EPT is induced by intramolecular charge-transfer (ICT) excitation of hydrogen-bonded-base adducts with either a coumarin dye or 4-nitro-4'-biphenylphenol. Femtosecond transient absorption spectralmore » measurements following ICT excitation reveal the appearance of two spectroscopically distinct states having different dynamical signatures. One of these states corresponds to a conventional ICT excited state in which the transferring H⁺ is initially associated with the proton donor. Proton transfer to the base (B) then occurs on the picosecond time scale. The other state is an ICT-EPT photoproduct. Upon excitation it forms initially in the nuclear configuration of the ground state by application of the Franck–Condon principle. However, due to the change in electronic configuration induced by the transition, excitation is accompanied by proton transfer with the protonated base formed with a highly elongated ⁺H–B bond. Coherent Raman spectroscopy confirms the presence of a vibrational mode corresponding to the protonated base in the optically prepared state.« less

Concerted electron-proton transfer in the optical excitation of hydrogen-bonded dyes.

PubMed

Westlake, Brittany C; Brennaman, M Kyle; Concepcion, Javier J; Paul, Jared J; Bettis, Stephanie E; Hampton, Shaun D; Miller, Stephen A; Lebedeva, Natalia V; Forbes, Malcolm D E; Moran, Andrew M; Meyer, Thomas J; Papanikolas, John M

2011-05-24

The simultaneous, concerted transfer of electrons and protons--electron-proton transfer (EPT)--is an important mechanism utilized in chemistry and biology to avoid high energy intermediates. There are many examples of thermally activated EPT in ground-state reactions and in excited states following photoexcitation and thermal relaxation. Here we report application of ultrafast excitation with absorption and Raman monitoring to detect a photochemically driven EPT process (photo-EPT). In this process, both electrons and protons are transferred during the absorption of a photon. Photo-EPT is induced by intramolecular charge-transfer (ICT) excitation of hydrogen-bonded-base adducts with either a coumarin dye or 4-nitro-4'-biphenylphenol. Femtosecond transient absorption spectral measurements following ICT excitation reveal the appearance of two spectroscopically distinct states having different dynamical signatures. One of these states corresponds to a conventional ICT excited state in which the transferring H(+) is initially associated with the proton donor. Proton transfer to the base (B) then occurs on the picosecond time scale. The other state is an ICT-EPT photoproduct. Upon excitation it forms initially in the nuclear configuration of the ground state by application of the Franck-Condon principle. However, due to the change in electronic configuration induced by the transition, excitation is accompanied by proton transfer with the protonated base formed with a highly elongated (+)H ─ B bond. Coherent Raman spectroscopy confirms the presence of a vibrational mode corresponding to the protonated base in the optically prepared state.

Probing Photoinduced Structural Phase Transitions by Fast or Ultra-Fast Time-Resolved X-Ray Diffraction

NASA Astrophysics Data System (ADS)

Cailleau, Hervé Collet, Eric; Buron-Le Cointe, Marylise; Lemée-Cailleau, Marie-Hélène Koshihara, Shin-Ya

A new frontier in the field of structural science is the emergence of the fast and ultra-fast X-ray science. Recent developments in time-resolved X-ray diffraction promise direct access to the dynamics of electronic, atomic and molecular motions in condensed matter triggered by a pulsed laser irradiation, i.e. to record "molecular movies" during the transformation of matter initiated by light pulse. These laser pump and X-ray probe techniques now provide an outstanding opportunity for the direct observation of a photoinduced structural phase transition as it takes place. The use of X-ray short-pulse of about 100ps around third-generation synchrotron sources allows structural investigations of fast photoinduced processes. Other new X-ray sources, such as laser-produced plasma ones, generate ultra-short pulses down to 100 fs. This opens the way to femtosecond X-ray crystallography, but with rather low X-ray intensities and more limited experimental possibilities at present. However this new ultra-fast science rapidly progresses around these sources and new large-scale projects exist. It is the aim of this contribution to overview the state of art and the perspectives of fast and ultra-fast X-ray scattering techniques to study photoinduced phase transitions (here, the word ultra-fast is used for sub-picosecond time resolution). In particular we would like to largely present the contribution of crystallographic methods in comparison with optical methods, such as pump-probe reflectivity measurements, the reader being not necessary familiar with X-ray scattering. Thus we want to present which type of physical information can be obtained from the positions of the Bragg peaks, their intensity and their shape, as well as from the diffuse scattering beyond Bragg peaks. An important physical feature is to take into consideration the difference in nature between a photoinduced phase transition and conventional homogeneous photoinduced chemical or biochemical processes where molecules transform in an independent way each other. Actually the photoinduced phase transition with the establishment of the new electronic and structural oscopic order is preceded by precursor co-operative phenomena due to the formation of nano-scale correlated objects. These are the counterpart of pre-transitional fluctuations at thermal equilibrium which take place above the transition temperature (short range order preceding long range one). Moreover ultra-fast X-ray scattering will play a central role within the fascinating field of manipulating coherence, for instance to directly observe coherent atomic motions induced by a light pulse, such as optical phonons. In the first part of this contribution we present what experimental features are accessible by X-ray scattering to describe the physical picture for a photoinduced structural phase transition. The second part shows how a time-resolved X-ray scattering experiment can be performed with regards to the different pulsed X-ray sources. The first time-resolved X-ray diffraction experiments on photoinduced phase transitions are described and discussed in the third part. Finally some challenges for future are briefly indicated in the conclusion.

Time-resolved structural dynamics of thin metal films heated with femtosecond optical pulses.

PubMed

Chen, Jie; Chen, Wei-Kan; Tang, Jau; Rentzepis, Peter M

2011-11-22

We utilize 100 fs optical pulses to induce ultrafast disorder of 35- to 150-nm thick single Au(111) crystals and observe the subsequent structural evolution using 0.6-ps, 8.04-keV X-ray pulses. Monitoring the picosecond time-dependent modulation of the X-ray diffraction intensity, width, and shift, we have measured directly electron/phonon coupling, phonon/lattice interaction, and a histogram of the lattice disorder evolution, such as lattice breath due to a pressure wave propagating at sonic velocity, lattice melting, and recrystallization, including mosaic formation. Results of theoretical simulations agree and support the experimental data of the lattice/liquid phase transition process. These time-resolved X-ray diffraction data provide a detailed description of all the significant processes induced by ultrafast laser pulses impinging on thin metallic single crystals.

Na2Ti6O13: a potential anode for grid-storage sodium-ion batteries.

PubMed

Rudola, Ashish; Saravanan, Kuppan; Devaraj, Sappani; Gong, Hao; Balaya, Palani

2013-08-28

The ultra-fast (30C or 2 min) rate capability and impressive long cycle life (>5000 cycles) of Na2Ti6O13 are reported. A stable 2.5 V sodium-ion battery full cell is demonstrated. In addition, the sodium storage mechanism and thermal stability of Na2Ti6O13 are discussed.

Carotid stiffness change over the cardiac cycle by ultrafast ultrasound imaging in healthy volunteers and vascular Ehlers-Danlos syndrome.

PubMed

Mirault, Tristan; Pernot, Mathieu; Frank, Michael; Couade, Mathieu; Niarra, Ralph; Azizi, Michel; Emmerich, Joseph; Jeunemaître, Xavier; Fink, Mathias; Tanter, Mickaël; Messas, Emmanuel

2015-09-01

Arterial stiffness is related to age and collagen properties of the arterial wall and can be indirectly evaluated by the pulse wave velocity (PWV). Ultrafast ultrasound imaging, a unique ultrahigh frame rate technique (>10, 000 images/s), recently emerged enabling direct measurement of carotid PWV and its variation over the cardiac cycle. Our goal was to characterize the carotid diastolic-systolic arterial stiffening using ultrafast ultrasound imaging in healthy individuals and in vascular Ehlers-Danlos syndrome (vEDS), in which collagen type III is defectuous. Ultrafast ultrasound imaging was performed on common carotids of 102 healthy individuals and 37 consecutive patients with vEDS. Results are mean ± standard deviation. Carotid ultrafast ultrasound imaging PWV in healthy individuals was 5.6 ± 1.2 in early systole and 7.3 ± 2.0  m/s in end systole, and correlated with age (r = 0.48; P < 0.0001 and r = 0.68; P < 0.0001, respectively). Difference between early and end-systole PWV increased with age independently of blood pressure (r = 0.54; P < 0.0001). In patients with vEDS, ultrafast ultrasound imaging PWV was 6.0 ± 1.5 in early systole and 6.7 ± 1.5  m/s in end systole. Carotid stiffness change over the cardiac cycle was lower than in healthy people (0.021 vs. 0.057  m/s per mmHg; P = 0.0035). Ultrafast ultrasound imaging can evaluate carotid PWV and its variation over the cardiac cycle. This allowed to demonstrate the age-induced increase of the arterial diastolic-systolic stiffening in healthy people and a lower stiffening in vEDS, both characterized by arterial complications. We believe that this easy-to-use technique could offer the opportunity to go beyond the diastolic PWV to better characterize arterial stiffness change with age or other collagen alterations.

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.

Ultrafast hopping dynamics of 5f electrons in the Mott insulator UO₂ studied by femtosecond pump-probe spectroscopy.

PubMed

An, Yong Q; Taylor, Antoinette J; Conradson, Steven D; Trugman, Stuart A; Durakiewicz, Tomasz; Rodriguez, George

2011-05-20

We describe a femtosecond pump-probe study of ultrafast hopping dynamics of 5f electrons in the Mott insulator UO₂ following Mott-gap excitation at temperatures of 5-300 K. Hopping-induced response of the lattice and electrons is probed by transient reflectivity at mid- and above-gap photon energies, respectively. These measurements show an instantaneous hop, subsequent picosecond lattice deformation, followed by acoustic phonon emission and microsecond relaxation. Temperature-dependent studies indicate that the slow relaxation results from Hubbard excitons formed by U³⁺-U⁵⁺ pairs.

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.

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.

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.

Unifying ultrafast demagnetization and intrinsic Gilbert damping in Co/Ni bilayers with electronic relaxation near the Fermi surface

NASA Astrophysics Data System (ADS)

Zhang, Wei; He, Wei; Zhang, Xiang-Qun; Cheng, Zhao-Hua; Teng, Jiao; Fähnle, Manfred

2017-12-01

The ability to controllably manipulate the laser-induced ultrafast magnetic dynamics is a prerequisite for future high-speed spintronic devices. The optimization of devices requires the controllability of the ultrafast demagnetization time τM and intrinsic Gilbert damping αintr. In previous attempts to establish a relationship between τM and αintr, the rare-earth doping of a permalloy film with two different demagnetization mechanisms was not a suitable candidate. Here, we choose Co/Ni bilayers to investigate the relations between τM and αintr by means of the time-resolved magneto-optical Kerr effect (TR-MOKE) via adjusting the thickness of the Ni layers, and obtain an approximately proportional relation between these two parameters. The remarkable agreement between the TR-MOKE experiment and the prediction of a breathing Fermi-surface model confirms that a large Elliott-Yafet spin-mixing parameter b2 is relevant to the strong spin-orbital coupling at the Co/Ni interface. More importantly, a proportional relation between τM and αintr in such metallic films or heterostructures with electronic relaxation near the Fermi surface suggests the local spin-flip scattering dominates the mechanism of ultrafast demagnetization, otherwise the spin-current mechanism dominates. It is an effective method to distinguish the dominant contributions to ultrafast magnetic quenching in metallic heterostructures by simultaneously investigating both the ultrafast demagnetization time and Gilbert damping. Our work can open an avenue to manipulate the magnitude and efficiency of terahertz emission in metallic heterostructures such as perpendicular magnetic anisotropic Ta/Pt/Co/Ni/Pt/Ta multilayers, and then it has an immediate implication for the design of high-frequency spintronic devices.

High Contrast Ultrafast Imaging of the Human Heart

PubMed Central

Papadacci, Clement; Pernot, Mathieu; Couade, Mathieu; Fink, Mathias; Tanter, Mickael

2014-01-01

Non-invasive ultrafast imaging for human cardiac applications is a big challenge to image intrinsic waves such as electromechanical waves or remotely induced shear waves in elastography imaging techniques. In this paper we propose to perform ultrafast imaging of the heart with adapted sector size by using diverging waves emitted from a classical transthoracic cardiac phased array probe. As in ultrafast imaging with plane wave coherent compounding, diverging waves can be summed coherently to obtain high-quality images of the entire heart at high frame rate in a full field-of-view. To image shear waves propagation at high SNR, the field-of-view can be adapted by changing the angular aperture of the transmitted wave. Backscattered echoes from successive circular wave acquisitions are coherently summed at every location in the image to improve the image quality while maintaining very high frame rates. The transmitted diverging waves, angular apertures and subapertures size are tested in simulation and ultrafast coherent compounding is implemented on a commercial scanner. The improvement of the imaging quality is quantified in phantom and in vivo on human heart. Imaging shear wave propagation at 2500 frame/s using 5 diverging waves provides a strong increase of the Signal to noise ratio of the tissue velocity estimates while maintaining a high frame rate. Finally, ultrafast imaging with a 1 to 5 diverging waves is used to image the human heart at a frame rate of 900 frames/s over an entire cardiac cycle. Thanks to spatial coherent compounding, a strong improvement of imaging quality is obtained with a small number of transmitted diverging waves and a high frame rate, which allows imaging the propagation of electromechanical and shear waves with good image quality. PMID:24474135

Non-thermal optical excitation of terahertz-spin precession in a magneto-optical insulator

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

Parchenko, Sergii; Maziewski, Andrzej; Stupakiewicz, Andrzej, E-mail: and@uwb.edu.pl

2016-01-18

We demonstrate non-thermal ultrafast laser excitation of spin precession with THz frequency in Gd-Bi-substituted iron garnet via the inverse Faraday effect. The modulation of THz precession by about 60 GHz below the compensation temperature of magnetic moment was observed. The THz frequency precession was caused by the exchange resonance between the Gd and Fe sublattices; we attributed the low-frequency modulation to dielectric resonance mode with a magnetic contribution. We demonstrate the possibility of polarization-sensitive control of spin precession under THz generation by laser pulses, helping to develop high-speed magneto-optical devices.

Effects of Current Guides Destruction at Ultra-fast Acceleration of Macrobodies

NASA Astrophysics Data System (ADS)

Kataev, V. N.; Boriskin, A. S.; Golosov, S. N.; Demidov, V. A.; Klimashov, M. V.; Korolev, P. V.; Makartsev, G. F.; Pikar, A. S.; Russkov, A. S.; Shapovalov, E. V.; Shibitov, Yu. M.

2006-08-01

The paper is devoted to discussion of current guides destruction effects in different accelerators: thermal-electric and electro-magnetic rail accelerator at macrobodies acceleration value of 108-109 m/s2. Experimental results with thermal-electric accelerators powering from megajoule capacitor battery and helical magneto-cumulative generator MCG-100 at currents up to 3.5 MA are analyzed. The process of rails destruction at railgun at pressure magnetic field excess over the limit of metal fluidity is presented. Methods of efficiency coefficient increase of capacitive storage energy transmission to kinetic energy of accelerating body are discussed.

Cooperative photoinduced metastable phase control in strained manganite films

NASA Astrophysics Data System (ADS)

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

2016-09-01

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

Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy

NASA Astrophysics Data System (ADS)

Guo, Zhi; Wan, Yan; Yang, Mengjin; Snaider, Jordan; Zhu, Kai; Huang, Libai

2017-04-01

The Shockley-Queisser limit for solar cell efficiency can be overcome if hot carriers can be harvested before they thermalize. Recently, carrier cooling time up to 100 picoseconds was observed in hybrid perovskites, but it is unclear whether these long-lived hot carriers can migrate long distance for efficient collection. We report direct visualization of hot-carrier migration in methylammonium lead iodide (CH3NH3PbI3) thin films by ultrafast transient absorption microscopy, demonstrating three distinct transport regimes. Quasiballistic transport was observed to correlate with excess kinetic energy, resulting in up to 230 nanometers transport distance that could overcome grain boundaries. The nonequilibrium transport persisted over tens of picoseconds and ~600 nanometers before reaching the diffusive transport limit. These results suggest potential applications of hot-carrier devices based on hybrid perovskites.

Nitrogen-Doped Holey Graphene Film-Based Ultrafast Electrochemical Capacitors.

PubMed

Zhou, Qinqin; Zhang, Miao; Chen, Ji; Hong, Jong-Dal; Shi, Gaoquan

2016-08-17

The commercialized aluminum electrolytic capacitors (AECs) currently used for alternating current (AC) line-filtering are usually the largest components in the electronic circuits because of their low specific capacitances and bulky sizes. Herein, nitrogen-doped holey graphene (NHG) films were prepared by thermal annealing the composite films of polyvinylpyrrolidone (PVP), graphene oxide (GO), and ferric oxide (Fe2O3) nanorods followed by chemical etching with hydrochloride acid. The typical electrochemical capacitor with NHG electrodes exhibited high areal and volumetric specific capacitances of 478 μF cm(-2) and 1.2 F cm(-3) at 120 Hz, ultrafast frequency response with a phase angle of -81.2° and a resistor-capacitor time constant of 203 μs at 120 Hz, as well as excellent cycling stability. Thus, it is promising to replace conventional AEC for AC line-filtering in miniaturized electronics.

Interferometer design and controls for pulse stacking in high power fiber lasers

NASA Astrophysics Data System (ADS)

Wilcox, Russell; Yang, Yawei; Dahlen, Dar; Xu, Yilun; Huang, Gang; Qiang, Du; Doolittle, Lawrence; Byrd, John; Leemans, Wim; Ruppe, John; Zhou, Tong; Sheikhsofla, Morteza; Nees, John; Galvanauskas, Almantas; Dawson, Jay; Chen, Diana; Pax, Paul

2017-03-01

In order to develop a design for a laser-plasma accelerator (LPA) driver, we demonstrate key technologies that enable fiber lasers to produce high energy, ultrafast pulses. These technologies must be scalable, and operate in the presence of thermal drift, acoustic noise, and other perturbations typical of an operating system. We show that coherent pulse stacking (CPS), which requires optical interferometers, can be made robust by image-relaying, multipass optical cavities, and by optical phase control schemes that sense pulse train amplitudes from each cavity. A four-stage pulse stacking system using image-relaying cavities is controlled for 14 hours using a pulse-pattern sensing algorithm. For coherent addition of simultaneous ultrafast pulses, we introduce a new scheme using diffractive optics, and show experimentally that four pulses can be added while a preserving pulse width of 128 fs.

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

Ultrafast Laser Interaction Processes for LIBS and Other Sensing Technologies

DTIC Science & Technology

2013-04-05

Propagation of ultrashort pulses through water, Optics Express, (02 2007): . doi: 12/02/2009 8.00 Z. Chen, S. Mao. Femtosecond laser -induced electronic...CO2 double- pulse laser -induced breakdown spectroscopy for explosive residues detection" SPIE Defense, Security, Sensing; Orlando, FL, USA; 04/07...Matthieu Baudelet, Michael Sigman, Paul J Dagdigian, Martin C. Richardson, "Nd:YAG-CO2 Double- Pulse Laser Induced Breakdown Spectroscopy for Explosive

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.

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.

Electron beam dynamics in an ultrafast transmission electron microscope with Wehnelt electrode.

PubMed

Bücker, K; Picher, M; Crégut, O; LaGrange, T; Reed, B W; Park, S T; Masiel, D J; Banhart, F

2016-12-01

High temporal resolution transmission electron microscopy techniques have shown significant progress in recent years. Using photoelectron pulses induced by ultrashort laser pulses on the cathode, these methods can probe ultrafast materials processes and have revealed numerous dynamic phenomena at the nanoscale. Most recently, the technique has been implemented in standard thermionic electron microscopes that provide a flexible platform for studying material's dynamics over a wide range of spatial and temporal scales. In this study, the electron pulses in such an ultrafast transmission electron microscope are characterized in detail. The microscope is based on a thermionic gun with a Wehnelt electrode and is operated in a stroboscopic photoelectron mode. It is shown that the Wehnelt bias has a decisive influence on the temporal and energy spread of the picosecond electron pulses. Depending on the shape of the cathode and the cathode-Wehnelt distance, different emission patterns with different pulse parameters are obtained. The energy spread of the pulses is determined by space charge and Boersch effects, given by the number of electrons in a pulse. However, filtering effects due to the chromatic aberrations of the Wehnelt electrode allow the extraction of pulses with narrow energy spreads. The temporal spread is governed by electron trajectories of different length and in different electrostatic potentials. High temporal resolution is obtained by excluding shank emission from the cathode and aberration-induced halos in the emission pattern. By varying the cathode-Wehnelt gap, the Wehnelt bias, and the number of photoelectrons in a pulse, tradeoffs between energy and temporal resolution as well as beam intensity can be made as needed for experiments. Based on the characterization of the electron pulses, the optimal conditions for the operation of ultrafast TEMs with thermionic gun assembly are elaborated. Copyright © 2016 Elsevier B.V. All rights reserved.

Scattering effects and high-spatial-frequency nanostructures on ultrafast laser irradiated surfaces of zirconium metallic alloys with nano-scaled topographies.

PubMed

Li, Chen; Cheng, Guanghua; Sedao, Xxx; Zhang, Wei; Zhang, Hao; Faure, Nicolas; Jamon, Damien; Colombier, Jean-Philippe; Stoian, Razvan

2016-05-30

The origin of high-spatial-frequency laser-induced periodic surface structures (HSFL) driven by incident ultrafast laser fields, with their ability to achieve structure resolutions below λ/2, is often obscured by the overlap with regular ripples patterns at quasi-wavelength periodicities. We experimentally demonstrate here employing defined surface topographies that these structures are intrinsically related to surface roughness in the nano-scale domain. Using Zr-based bulk metallic glass (Zr-BMG) and its crystalline alloy (Zr-CA) counterpart formed by thermal annealing from its glassy precursor, we prepared surfaces showing either smooth appearances on thermoplastic BMG or high-density nano-protuberances from randomly distributed embedded nano-crystallites with average sizes below 200 nm on the recrystallized alloy. Upon ultrashort pulse irradiation employing linearly polarized 50 fs, 800 nm laser pulses, the surfaces show a range of nanoscale organized features. The change of topology was then followed under multiple pulse irradiation at fluences around and below the single pulse threshold. While the former material (Zr-BMG) shows a specific high quality arrangement of standard ripples around the laser wavelength, the latter (Zr-CA) demonstrates strong predisposition to form high spatial frequency rippled structures (HSFL). We discuss electromagnetic scenarios assisting their formation based on near-field interaction between particles and field-enhancement leading to structure linear growth. Finite-difference-time-domain simulations outline individual and collective effects of nanoparticles on electromagnetic energy modulation and the feedback processes in the formation of HSFL structures with correlation to regular ripples (LSFL).

Energy & Energetics

DTIC Science & Technology

2012-06-22

mechanical and structural failure and decomposition in ultra-fast time regimes. Our research teams are exploring novel ways to convert mechanical ...energy to thermal energy by examining initiation mechanisms , multi-phase combustion, detonation and the mechanisms that lead to the release of energy...understanding of the mechanisms of structural stability by doping Fe in LiCoPO4 and effectiveness of HFiP in stopping further oxidation of electrolytes are

Research@ARL: Energy & Energetics

DTIC Science & Technology

2012-06-01

enabling us to probe chemical, mechanical and structural failure and decomposition in ultra-fast time regimes. Our research teams are exploring novel ways...to convert mechanical energy to thermal energy by examining initiation mechanisms , multi-phase combustion, detonation and the mechanisms that lead...storage life. The understanding of the mechanisms of structural stability by doping Fe in LiCoPO4 and effectiveness of HFiP in stopping further

Precision resection of lung cancer in a sheep model using ultrashort laser pulses

NASA Astrophysics Data System (ADS)

Beck, Rainer J.; Mohanan, Syam Mohan P. C.; Góra, Wojciech S.; Cousens, Chris; Finlayson, Jeanie; Dagleish, Mark P.; Griffiths, David J.; Shephard, Jonathan D.

2017-02-01

Recent developments and progress in the delivery of high average power ultrafast laser pulses enable a range of novel minimally invasive surgical procedures. Lung cancer is the leading cause of cancer deaths worldwide and here the resection of lung tumours by means of picosecond laser pulses is presented. This represents a potential alternative to mitigate limitations of existing surgical treatments in terms of precision and collateral thermal damage to the healthy tissue. Robust process parameters for the laser resection are demonstrated using ovine pulmonary adenocarcinoma (OPA). OPA is a naturally occurring lung cancer of sheep caused by retrovirus infection that has several features in common with some forms of human pulmonary adenocarcinoma, including a similar histological appearance, which makes it ideally suited for this study. The picosecond laser was operated at a wavelength of 515 nm to resect square cavities from fresh ex-vivo OPA samples using a range of scanning strategies. Process parameters are presented for efficient ablation of the tumour with clear margins and only minimal collateral damage to the surrounding tissue. The resection depth can be controlled precisely by means of the pulse energy. By adjusting the overlap between successive laser pulses, deliberate heat transfer to the tissue and thermal damage can be achieved. This can be beneficial for on demand haemostasis and laser coagulation. Overall, the application of ultrafast lasers for the resection of lung tumours has potential to enable significantly improved precision and reduced thermal damage to the surrounding tissue compared to conventional techniques.

Ultrafast magnetization modulation induced by the electric field component of a terahertz pulse in a ferromagnetic-semiconductor thin film.

PubMed

Ishii, Tomoaki; Yamakawa, Hiromichi; Kanaki, Toshiki; Miyamoto, Tatsuya; Kida, Noriaki; Okamoto, Hiroshi; Tanaka, Masaaki; Ohya, Shinobu

2018-05-02

High-speed magnetization control of ferromagnetic films using light pulses is attracting considerable attention and is increasingly important for the development of spintronic devices. Irradiation with a nearly monocyclic terahertz pulse, which can induce strong electromagnetic fields in ferromagnetic films within an extremely short time of less than ~1 ps, is promising for damping-free high-speed coherent control of the magnetization. Here, we successfully observe a terahertz response in a ferromagnetic-semiconductor thin film. In addition, we find that a similar terahertz response is observed even in a non-magnetic semiconductor and reveal that the electric-field component of the terahertz pulse plays a crucial role in the magnetization response through the spin-carrier interactions in a ferromagnetic-semiconductor thin film. Our findings will provide new guidelines for designing materials suitable for ultrafast magnetization reversal.

Role of coherence and delocalization in photo-induced electron transfer at organic interfaces

NASA Astrophysics Data System (ADS)

Abramavicius, V.; Pranculis, V.; Melianas, A.; Inganäs, O.; Gulbinas, V.; Abramavicius, D.

2016-09-01

Photo-induced charge transfer at molecular heterojunctions has gained particular interest due to the development of organic solar cells (OSC) based on blends of electron donating and accepting materials. While charge transfer between donor and acceptor molecules can be described by Marcus theory, additional carrier delocalization and coherent propagation might play the dominant role. Here, we describe ultrafast charge separation at the interface of a conjugated polymer and an aggregate of the fullerene derivative PCBM using the stochastic Schrödinger equation (SSE) and reveal the complex time evolution of electron transfer, mediated by electronic coherence and delocalization. By fitting the model to ultrafast charge separation experiments, we estimate the extent of electron delocalization and establish the transition from coherent electron propagation to incoherent hopping. Our results indicate that even a relatively weak coupling between PCBM molecules is sufficient to facilitate electron delocalization and efficient charge separation at organic interfaces.

Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response

DOE PAGES

Kohler, Daniel D.; Thompson, Blaise J.; Wright, John C.

2017-08-31

Ultrafast spectroscopy is often collected in the mixed frequency/time domain, where pulse durations are similar to system dephasing times. In these experiments, expectations derived from the familiar driven and impulsive limits are not valid. This work simulates the mixed-domain four-wave mixing response of a model system to develop expectations for this more complex field-matter interaction. We also explore frequency and delay axes. We show that these line shapes are exquisitely sensitive to excitation pulse widths and delays. Near pulse overlap, the excitation pulses induce correlations that resemble signatures of dynamic inhomogeneity. We describe these line shapes using an intuitive picturemore » that connects to familiar field-matter expressions. We develop strategies for distinguishing pulse-induced correlations from true system inhomogeneity. Our simulations provide a foundation for interpretation of ultrafast experiments in the mixed domain.« less

Mapping molecular motions leading to charge delocalization with ultrabright electrons

NASA Astrophysics Data System (ADS)

Sciaini, German

2014-05-01

Ultrafast diffraction has broken the barrier to atomic exploration by combining the atomic spatial resolution of diffraction techniques with the temporal resolution of ultrafast spectroscopy. X-ray free electron lasers, slicing techniques and femtosecond laser-driven X-ray and electron sources have been successfully applied for the study of ultrafast structural dynamics in a variety of samples. Yet, the application of fs-diffraction to the study of rather sensitive organic molecular crystals remains unexplored. Organic crystals are composed by weak scattering centres, often present low melting points, poor heat conductivity and are, typically, radiation sensitive. Low repetition rates (about tens of Hertz) are therefore required to overcome accumulative heating effects from the laser excitation that can degrade the sample and mask the structural dynamics. This imparts tremendous constraints on source brightness to acquire enough diffraction data before adverse photo-degradation effects have played a non-negligible role in the crystalline structure. We implemented ultra-bright femtosecond electron diffraction to obtain a movie of the relevant molecular motions driving the photo-induced insulator-to-metal phase transition in the organic charge-transfer salt (EDO-TTF)2PF6. On the first few picoseconds (0 - 10 ps) the structural evolution, well-described by three main reaction coordinates, reaches a transient intermediate state (TIS). Model structural refinement calculations indicate that fast sliding of flat EDO-TTF molecules with consecutive motion of PF6 counter-ions drive the formation of TS instead of the expected flattening of initially bent EDO-TTF moieties which seems to evolve through a slower thermal pathway that brings the system into a final high temperature-type state. These findings establish the potential of ultrabright femtosecond electron sources for probing the primary processes governing structural dynamics with atomic resolution in labile systems relevant to chemistry and biology. For more information vide-infra Gao et al., Funding for this project was provided by the Natural Sciences and Engineering Research Council of Canada and the Canada Foundation for Innovation and Grant Agencies in Japan, vide infra Nature reference for more details.

Desolvation of polymers by ultrafast heating: Influence of hydrophilicity

NASA Astrophysics Data System (ADS)

Sun, Si Neng; Urbassek, Herbert M.

2010-10-01

Using molecular-dynamics simulation, we investigate the consequences of ultrafast laser-induced heating of a small water droplet containing a solvated polymer. Two polymers are studied: polyethylene as an example of a hydrophobic, and polyketone as an example of a hydrophilic polymer. In both cases, when the droplet is heated below the critical temperature of water, strong water evaporation is started, but the polymer remains in contact with a central water cluster. However, upon heating beyond the critical temperature, the hydrophilic polyethylene becomes completely desolvated, while polyketone still remains solvated. We analyze this behavior in terms of the intermolecular interactions and of the expansion dynamics of the heated droplet.

Higgs amplitude mode in the BCS superconductors Nb1-xTi(x)N induced by terahertz pulse excitation.

PubMed

Matsunaga, Ryusuke; Hamada, Yuki I; Makise, Kazumasa; Uzawa, Yoshinori; Terai, Hirotaka; Wang, Zhen; Shimano, Ryo

2013-08-02

Ultrafast responses of BCS superconductor Nb(1-x)Ti(x)N films in a nonadiabatic excitation regime were investigated by using terahertz (THz) pump-THz probe spectroscopy. After an instantaneous excitation with the monocycle THz pump pulse, a transient oscillation emerges in the electromagnetic response in the BCS gap energy region. The oscillation frequency coincides with the asymptotic value of the BCS gap energy, indicating the appearance of the theoretically anticipated collective amplitude mode of the order parameter, namely the Higgs amplitude mode. Our result opens a new pathway to the ultrafast manipulation of the superconducting order parameter by optical means.

Ultrashort electron pulses as a four-dimensional diagnosis of plasma dynamics.

PubMed

Zhu, P F; Zhang, Z C; Chen, L; Li, R Z; Li, J J; Wang, X; Cao, J M; Sheng, Z M; Zhang, J

2010-10-01

We report an ultrafast electron imaging system for real-time examination of ultrafast plasma dynamics in four dimensions. It consists of a femtosecond pulsed electron gun and a two-dimensional single electron detector. The device has an unprecedented capability of acquiring a high-quality shadowgraph image with a single ultrashort electron pulse, thus permitting the measurement of irreversible processes using a single-shot scheme. In a prototype experiment of laser-induced plasma of a metal target under moderate pump intensity, we demonstrated its unique capability of acquiring high-quality shadowgraph images on a micron scale with a-few-picosecond time resolution.

Noise Equalization for Ultrafast Plane Wave Microvessel Imaging.

PubMed

Song, Pengfei; Manduca, Armando; Trzasko, Joshua D; Chen, Shigao

2017-11-01

Ultrafast plane wave microvessel imaging significantly improves ultrasound Doppler sensitivity by increasing the number of Doppler ensembles that can be collected within a short period of time. The rich spatiotemporal plane wave data also enable more robust clutter filtering based on singular value decomposition. However, due to the lack of transmit focusing, plane wave microvessel imaging is very susceptible to noise. This paper was designed to: 1) study the relationship between ultrasound system noise (primarily time gain compensation induced) and microvessel blood flow signal and 2) propose an adaptive and computationally cost-effective noise equalization method that is independent of hardware or software imaging settings to improve microvessel image quality.

Ultrafast laser control of backward superfluorescence towards standoff sensing

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

Ariunbold, Gombojav O.; National University of Mongolia, Ulaanbaatar 210646; Baylor University, Waco, Texas 76798

2014-01-13

We study infrared backward cooperative emission in a rubidium vapor induced by ultrafast two-photon optical excitations. The laser coherent control of the backward emission is demonstrated by using a pair of 100 fs pulses with a variable time delay. The temporal variation (quantum beat) of the backward beam intensity due to interference of atomic transitions in the rubidium atomic level system 5S-5P-5D is produced and controlled. Based on the obtained experimental results, we discuss possible applications of the developed approach for creation of an effective “guide star” in the sodium atomic layer in the upper atmosphere (mesosphere)

Extremely Black Vertically Aligned Carbon Nanotube Arrays for Solar Steam Generation.

PubMed

Yin, Zhe; Wang, Huimin; Jian, Muqiang; Li, Yanshen; Xia, Kailun; Zhang, Mingchao; Wang, Chunya; Wang, Qi; Ma, Ming; Zheng, Quan-Shui; Zhang, Yingying

2017-08-30

The unique structure of a vertically aligned carbon nanotube (VACNT) array makes it behave most similarly to a blackbody. It is reported that the optical absorptivity of an extremely black VACNT array is about 0.98-0.99 over a large spectral range of 200 nm-200 μm, inspiring us to explore the performance of VACNT arrays in solar energy harvesting. In this work, we report the highly efficient steam generation simply by laminating a layer of VACNT array on the surface of water to harvest solar energy. It is found that under solar illumination the temperature of upper water can significantly increase with obvious water steam generated, indicating the efficient solar energy harvesting and local temperature rise by the thin layer of VACNTs. We found that the evaporation rate of water assisted by VACNT arrays is 10 times that of bare water, which is the highest ratio for solar-thermal-steam generation ever reported. Remarkably, the solar thermal conversion efficiency reached 90%. The excellent performance could be ascribed to the strong optical absorption and local temperature rise induced by the VACNT layer, as well as the ultrafast water transport through the VACNT layer due to the frictionless wall of CNTs. Based on the above, we further demonstrated the application of VACNT arrays in solar-driven desalination.

Optical and thermal properties in ultrafast laser surface nanostructuring on biodegradable polymer

NASA Astrophysics Data System (ADS)

Yada, Shuhei; Terakawa, Mitsuhiro

2015-03-01

We investigate the effect of optical and thermal properties in laser-induced periodic surface structures (LIPSS) formation on a poly-L-lactic acid (PLLA), a biodegradable polymer. Surface properties of biomaterials are known to be one of the key factors in tissue engineering. Methods to process biomaterial surfaces have been studied widely to enhance cell adhesive and anisotropic properties. LIPSS formation has advantages in a dry processing which is able to process complex-shaped surfaces without using a toxic chemical component. LIPSS, however, was difficult to be formed on PLLA due to its thermal and optical properties compared to other polymers. To obtain new perspectives in effect of these properties above, LIPSS formation dependences on wavelength, pulse duration and repetition rate have been studied. At 800 nm of incident wavelength, high-spatial frequency LIPSS (HSFL) was formed after applying 10000 femtosecond pulses at 1.0 J/cm2 in laser fluence. At 400 nm of the wavelength, HSFL was formed at fluences higher than 0.20 J/cm2 with more than 3000 pulses. Since LIPSS was less formed with lower repetition rate, certain heat accumulation may be required for LIPSS formation. With the pulse duration of 2.0 ps, higher laser fluence as well as number of pulses compared to the case of 120 fs was necessary. This indicates that multiphoton absorption process is essential for LIPSS formation. Study on biodegradation modification was also performed.

Ultrafast magnetization switching by spin-orbit torques

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

Garello, Kevin, E-mail: kevin.garello@mat.ethz.ch; Avci, Can Onur; Baumgartner, Manuel

2014-11-24

Spin-orbit torques induced by spin Hall and interfacial effects in heavy metal/ferromagnetic bilayers allow for a switching geometry based on in-plane current injection. Using this geometry, we demonstrate deterministic magnetization reversal by current pulses ranging from 180 ps to ms in Pt/Co/AlO{sub x} dots with lateral dimensions of 90 nm. We characterize the switching probability and critical current I{sub c} as a function of pulse length, amplitude, and external field. Our data evidence two distinct regimes: a short-time intrinsic regime, where I{sub c} scales linearly with the inverse of the pulse length, and a long-time thermally assisted regime, where I{sub c} variesmore » weakly. Both regimes are consistent with magnetization reversal proceeding by nucleation and fast propagation of domains. We find that I{sub c} is a factor 3–4 smaller compared to a single domain model and that the incubation time is negligibly small, which is a hallmark feature of spin-orbit torques.« less

Liquid-like thermal conduction in intercalated layered crystalline solids

DOE PAGES

Li, B.; Wang, H.; Kawakita, Y.; ...

2018-01-15

As a generic property, all substances transfer heat through microscopic collisions of constituent particles. A solid conducts heat through both transverse and longitudinal acoustic phonons, but a liquid employs only longitudinal vibrations. As a result, a solid is usually thermally more conductive than a liquid. In canonical viewpoints, such a difference also serves as the dynamic signature distinguishing a solid from a liquid. Here in this work, we report liquid-like thermal conduction observed in the crystalline AgCrSe 2. The transverse acoustic phonons are completely suppressed by the ultrafast dynamic disorder while the longitudinal acoustic phonons are strongly scattered but survive,more » and are thus responsible for the intrinsically ultralow thermal conductivity. This scenario is applicable to a wide variety of layered compounds with heavy intercalants in the van der Waals gaps, manifesting a broad implication on suppressing thermal conduction. Finally, these microscopic insights might reshape the fundamental understanding on thermal transport properties of matter and open up a general opportunity to optimize performances of thermoelectrics.« less

Liquid-like thermal conduction in intercalated layered crystalline solids

NASA Astrophysics Data System (ADS)

Li, B.; Wang, H.; Kawakita, Y.; Zhang, Q.; Feygenson, M.; Yu, H. L.; Wu, D.; Ohara, K.; Kikuchi, T.; Shibata, K.; Yamada, T.; Ning, X. K.; Chen, Y.; He, J. Q.; Vaknin, D.; Wu, R. Q.; Nakajima, K.; Kanatzidis, M. G.

2018-03-01

As a generic property, all substances transfer heat through microscopic collisions of constituent particles1. A solid conducts heat through both transverse and longitudinal acoustic phonons, but a liquid employs only longitudinal vibrations2,3. As a result, a solid is usually thermally more conductive than a liquid. In canonical viewpoints, such a difference also serves as the dynamic signature distinguishing a solid from a liquid. Here, we report liquid-like thermal conduction observed in the crystalline AgCrSe2. The transverse acoustic phonons are completely suppressed by the ultrafast dynamic disorder while the longitudinal acoustic phonons are strongly scattered but survive, and are thus responsible for the intrinsically ultralow thermal conductivity. This scenario is applicable to a wide variety of layered compounds with heavy intercalants in the van der Waals gaps, manifesting a broad implication on suppressing thermal conduction. These microscopic insights might reshape the fundamental understanding on thermal transport properties of matter and open up a general opportunity to optimize performances of thermoelectrics.

Liquid-like thermal conduction in intercalated layered crystalline solids

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

Li, B.; Wang, H.; Kawakita, Y.

As a generic property, all substances transfer heat through microscopic collisions of constituent particles. A solid conducts heat through both transverse and longitudinal acoustic phonons, but a liquid employs only longitudinal vibrations. As a result, a solid is usually thermally more conductive than a liquid. In canonical viewpoints, such a difference also serves as the dynamic signature distinguishing a solid from a liquid. Here in this work, we report liquid-like thermal conduction observed in the crystalline AgCrSe 2. The transverse acoustic phonons are completely suppressed by the ultrafast dynamic disorder while the longitudinal acoustic phonons are strongly scattered but survive,more » and are thus responsible for the intrinsically ultralow thermal conductivity. This scenario is applicable to a wide variety of layered compounds with heavy intercalants in the van der Waals gaps, manifesting a broad implication on suppressing thermal conduction. Finally, these microscopic insights might reshape the fundamental understanding on thermal transport properties of matter and open up a general opportunity to optimize performances of thermoelectrics.« less

Dynamics of Carotenoids Probed by Femtosecond Absorption, Fluorescence, and Raman Spectroscopy

NASA Astrophysics Data System (ADS)

Yoshizawa, M.; Kosumi, D.; Komukai, M.; Yanagi, K.; Hashimoto, H.

Ultrafast optical responses in β-carotene and lycopene depend on the pump wavelength. Excess vibrational energy induced by the photoexcitation remains longer than several picoseconds in the excited states and slows down the relaxation kinetics.

Direct characterization of photoinduced lattice dynamics in BaFe 2As 2

DOE PAGES

Gerber, S.; Kim, K. W.; Zhang, Y.; ...

2015-06-08

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe 2As 2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent latticemore » dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands.« less

Direct characterization of photoinduced lattice dynamics in BaFe2As2

PubMed Central

Gerber, S.; Kim, K. W.; Zhang, Y.; Zhu, D.; Plonka, N.; Yi, M.; Dakovski, G. L.; Leuenberger, D.; Kirchmann, P.S.; Moore, R. G.; Chollet, M.; Glownia, J. M.; Feng, Y.; Lee, J.-S.; Mehta, A.; Kemper, A. F.; Wolf, T.; Chuang, Y.-D.; Hussain, Z.; Kao, C.-C.; Moritz, B.; Shen, Z.-X.; Devereaux, T. P.; Lee, W.-S.

2015-01-01

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe2As2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent lattice dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands. PMID:26051704

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

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.

Non-stochastic reprogramming from a privileged somatic cell state

PubMed Central

Guo, Shangqin; Zi, Xiaoyuan; Schulz, Vincent P.; Cheng, Jijun; Zhong, Mei; Koochaki, Sebastian H.J.; Megyola, Cynthia M.; Pan, Xinghua; Heydari, Kartoosh; Weissman, Sherman M.; Gallagher, Patrick G.; Krause, Diane S.; Fan, Rong; Lu, Jun

2014-01-01

SUMMARY Reprogramming somatic cells to induced pluripotency by Yamanaka factors is usually slow and inefficient, and is thought to be a stochastic process. We identified a privileged somatic cell state, from which acquisition of pluripotency could occur in a non-stochastic manner. Subsets of murine hematopoietic progenitors are privileged, whose progeny cells predominantly adopt the pluripotent fate with activation of endogenous Oct4 locus after 4–5 divisions in reprogramming conditions. Privileged cells display an ultrafast cell cycle of ~8 hours. In fibroblasts, a subpopulation cycling at a similar ultrafast speed is observed after 6 days of factor expression, and is increased by p53-knockdown. This ultrafast-cycling population accounts for >99% of the bulk reprogramming activity in wildtype or p53-knockdown fibroblasts. Our data demonstrate that the stochastic nature of reprogramming can be overcome in a privileged somatic cell state, and suggest that cell cycle acceleration toward a critical threshold is an important bottleneck for reprogramming. PMID:24486105

THz-driven demagnetization with perpendicular magnetic anisotropy: towards ultrafast ballistic switching

NASA Astrophysics Data System (ADS)

Polley, Debanjan; Pancaldi, Matteo; Hudl, Matthias; Vavassori, Paolo; Urazhdin, Sergei; Bonetti, Stefano

2018-02-01

We study THz-driven spin dynamics in thin CoPt films with perpendicular magnetic anisotropy. Femtosecond magneto-optical Kerr effect measurements show that demagnetization amplitude of about 1% can be achieved with a peak THz electric field of 300 kV cm-1, and a corresponding peak magnetic field of 0.1 T. The effect is more than an order of magnitude larger than observed in samples with easy-plane anisotropy irradiated with the same field strength. We also utilize finite-element simulations to design a meta-material structure that can enhance the THz magnetic field by more than an order of magnitude, over an area of several tens of square micrometers. Magnetic fields exceeding 1 Tesla, generated in such meta-materials with the available laser-based THz sources, are expected to produce full magnetization reversal via ultrafast ballistic precession driven by the THz radiation. Our results demonstrate the possibility of table-top ultrafast magnetization reversal induced by THz radiation.

Self-amplified photo-induced gap quenching in a correlated electron material

DOE PAGES

Mathias, S.; Eich, S.; Urbancic, J.; ...

2016-10-04

Capturing the dynamic electronic band structure of a correlated material presents a powerful capability for uncovering the complex couplings between the electronic and structural degrees of freedom. When combined with ultrafast laser excitation, new phases of matter can result, since far-from-equilibrium excited states are instantaneously populated. Here, we elucidate a general relation between ultrafast non-equilibrium electron dynamics and the size of the characteristic energy gap in a correlated electron material. Here, we show that carrier multiplication via impact ionization can be one of the most important processes in a gapped material, and that the speed of carrier multiplication critically dependsmore » on the size of the energy gap. In the case of the charge-density wave material 1T-TiSe 2, our data indicate that carrier multiplication and gap dynamics mutually amplify each other, which explains—on a microscopic level—the extremely fast response of this material to ultrafast optical excitation.« 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

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.

Alternative Electron-Transfer Channels Ensure Ultrafast Deactivation of Light-Induced Excited States in Riboflavin Binding Protein.

PubMed

Zanetti-Polzi, Laura; Aschi, Massimiliano; Amadei, Andrea; Daidone, Isabella

2017-07-20

Flavoproteins, containing flavin chromophores, are enzymes capable of transferring electrons at very high speeds. The ultrafast photoinduced electron-transfer (ET) kinetics of riboflavin binding protein to the excited riboflavin was studied by femtosecond spectroscopy and found to occur within a few hundred femtoseconds [ Zhong and Zewail, Proc. Natl. Acad. Sci. U.S.A. 2001, 98, 11867-11872 ]. This ultrafast kinetics was attributed to the presence of two aromatic rings that could transfer the electron to riboflavin: the side chains of tryptophan 156 and tyrosine 75. However, the underlying ET mechanism remained unclear. Here, using a hybrid quantum mechanical-molecular dynamics approach, we perform ET dynamics simulations taking into account the motion of the protein and the solvent upon ET. This approach reveals that ET occurs via a major reaction channel involving tyrosine 75 (83%) and a minor one involving tryptophan 156 (17%). We also show that the protein environment is designed to ensure the fast quenching of the riboflavin excited state.

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 strong-field photoelectron emission from biased metal surfaces: exact solution to time-dependent Schrödinger Equation

PubMed Central

Zhang, Peng; Lau, Y. Y.

2016-01-01

Laser-driven ultrafast electron emission offers the possibility of manipulation and control of coherent electron motion in ultrashort spatiotemporal scales. Here, an analytical solution is constructed for the highly nonlinear electron emission from a dc biased metal surface illuminated by a single frequency laser, by solving the time-dependent Schrödinger equation exactly. The solution is valid for arbitrary combinations of dc electric field, laser electric field, laser frequency, metal work function and Fermi level. Various emission mechanisms, such as multiphoton absorption or emission, optical or dc field emission, are all included in this single formulation. The transition between different emission processes is analyzed in detail. The time-dependent emission current reveals that intense current modulation may be possible even with a low intensity laser, by merely increasing the applied dc bias. The results provide insights into the electron pulse generation and manipulation for many novel applications based on ultrafast laser-induced electron emission. PMID:26818710

In vivo studies of ultrafast near-infrared laser tissue bonding and wound healing

PubMed Central

Sriramoju, Vidyasagar; Alfano, Robert R.

2015-01-01

Abstract. Femtosecond (fs) pulse lasers in the near-infrared (NIR) range exhibit very distinct properties upon their interaction with biomolecules compared to the corresponding continuous wave (CW) lasers. Ultrafast NIR laser tissue bonding (LTB) was used to fuse edges of two opposing animal tissue segments in vivo using fs laser photoexcitation of the native vibrations of chomophores. The fusion of the incised tissues was achieved in vivo at the molecular level as the result of the energy–matter interactions of NIR laser radiation with water and the structural proteins like collagen in the target tissues. Nonthermal vibrational excitation from the fs laser absorption by water and collagen induced the formation of cross-links between tissue proteins on either sides of the weld line resulting in tissue bonding. No extrinsic agents were used to facilitate tissue bonding in the fs LTB. These studies were pursued for the understanding and evaluation of the role of ultrafast NIR fs laser radiation in the LTB and consequent wound healing. The fs LTB can be used for difficult to suture structures such as blood vessels, nerves, gallbladder, liver, intestines, and other viscera. Ultrafast NIR LTB yields promising outcomes and benefits in terms of wound closure and wound healing under optimal conditions. PMID:26465615

In vivo studies of ultrafast near-infrared laser tissue bonding and wound healing

NASA Astrophysics Data System (ADS)

Sriramoju, Vidyasagar; Alfano, Robert R.

2015-10-01

Femtosecond (fs) pulse lasers in the near-infrared (NIR) range exhibit very distinct properties upon their interaction with biomolecules compared to the corresponding continuous wave (CW) lasers. Ultrafast NIR laser tissue bonding (LTB) was used to fuse edges of two opposing animal tissue segments in vivo using fs laser photoexcitation of the native vibrations of chomophores. The fusion of the incised tissues was achieved in vivo at the molecular level as the result of the energy-matter interactions of NIR laser radiation with water and the structural proteins like collagen in the target tissues. Nonthermal vibrational excitation from the fs laser absorption by water and collagen induced the formation of cross-links between tissue proteins on either sides of the weld line resulting in tissue bonding. No extrinsic agents were used to facilitate tissue bonding in the fs LTB. These studies were pursued for the understanding and evaluation of the role of ultrafast NIR fs laser radiation in the LTB and consequent wound healing. The fs LTB can be used for difficult to suture structures such as blood vessels, nerves, gallbladder, liver, intestines, and other viscera. Ultrafast NIR LTB yields promising outcomes and benefits in terms of wound closure and wound healing under optimal conditions.

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

The Evolution of Surface Symmetry in Femtosecond Laser-Induced Transient States of Matter

NASA Astrophysics Data System (ADS)

Garnett, Joy Carleen

Gallium arsenide and other III-V materials are well known for their excellent optical and electronic properties and have led to the development of high-performance photovoltaic cells1,2, photoelectrochemical water splitting3,4, and light emitting diodes (LEDs)5. Several combinations of III-V semiconductors are now being considered as potentially attractive alternatives to silicon for these applications. However, further development requires fundamental understanding of processes that govern light-matter interactions. Specifically, surface strain and ultrafast dynamics are of great interest to the optoelectronic industry. Strained semiconductor surfaces dominate the design of optoelectronics and III-V semiconductor-based LEDs. Currently, the structures of strained surfaces are well characterized with x-ray diffraction (XRD)6 and electron crystallography7-9. However, optically-induced electronic behavior at these interfaces are not fully understood. This has the been one of the stimulants for the research in this dissertation. To further explore opticallyinduced electronic behavior at strained interfaces, I have asked the following questions: 1. How does static optoelectronic behavior change as a function of strain? 2. How does surface symmetry and electronic motion change with respect to strain? 3. How do atomic bonds change as a function of strain? Another main research goal of this work is to understand ultrafast subpicosecond processes after pulsed laser excitation. The knowledge of ultrafast processes dominates the design of devices in industries that require high temporal and spectral resolution. Ultrafast atomic motion has been the major focus of subpicosecond structural dynamics. Currently, these dynamics upon photoexcitation are well characterized with experimental methods such as ultrafast x-ray diffraction (U-XRD), ultrafast electron diffraction (UED), and ultrafast electron crystallography (UEC). However, ultrafast atomic motion does not occur alone. The bonds connecting these moving atoms are also affected during this process. The correlation between structural and electronic dynamics is not well understood. To further explore correlated structural and electronic behavior upon ultrafast laser excitation, I have asked the following questions: 1. How does subpicosecond optoelectronic behavior change as a function of time after femtosecond pulse photoexcitation? 2. How does subpicosecond surface symmetry and electronic motion change with respect to time after femtosecond pulse photoexcitation? 3. How do atomic bonds change as a function of time after femtosecond pulse photoexcitation? To address these questions, I used experimental methods sensitive to both atomic motions and electronic responses: polarization-resolved second harmonic generation (PRSHG) and timeresolved, polarization-resolved second harmonic generation (TRPRSHG). The dissertation covers application of these techniques to III-V semiconductors: gallium arsenide (GaAs), gallium antimonide (GaSb), and aluminum gallium arsenide (AlGaAs). This dissertation is organized as follows. Chapter 2 presents the background of electronic band structures, ultrafast relaxation processes, and the origin of nonlinear optics from the perspectives of classical and quantum mechanics. It thus provides a framework for the static and transient nonlinear optical processes observed in III-V semiconductors under ultrafast pulse excitation. Next, Chapter 3 motivates the use of the experimental and analytical methods as applied to the experimental and theoretical studies outlined in Chapters 4 and 5. Chapter 4 is devoted to the understanding of polarization-resolved second-order nonlinear optical responses of various strained III-V semiconductor heterostructures resulting from defect-conducive growth conditions. Simplified phenomenological expressions for the polarization-resolved second harmonic generation (PRSHG) are first derived using tensor analysis. Afterwards, these expressions are used to fit experimental data. The developed formalism is tested under different conditions to gauge the fit robustness and sensitivity to mechanical and electronic changes in strained IIIV semiconductors. Along that same vein, Chapter 5 extends this analytical fit to describe ultrafast PRSHG responses of GaAs (100) as a function of transient changes in the interatomic potential within the first picosecond after photoexcitation. Finally, the dissertation concludes with Chapter 6 addressing possible directions for future work. The chapter begins with a description of studies to further test the sensitivity and robustness of the PRSHG phenomenological fit and how it can be used to characterize more classes of materials.

EDITORIAL: Ultrafast magnetization processes

NASA Astrophysics Data System (ADS)

Hillebrands, Burkard

2008-09-01

This Cluster Issue of Journal of Physics D: Applied Physics is devoted to ultrafast magnetization processes. It reports on the scientific yield of the Priority Programme 1133 'Ultrafast Magnetization Processes' which was funded by the Deutsche Forschungsgemeinschaft in the period 2002-2008 in three successive two-year funding periods, supporting research of 17-18 groups in Germany. Now, at the end of this Priority Programme, the members feel that the achievements made in the course of the programme merit communication to the international scientific community in a concerted way. Therefore, each of the projects of the last funding period presents a key result in a published contribution to this Cluster Issue. The purpose of the funding by a Priority Programme is to advance knowledge in an emerging field of research through collaborative networked support over several locations. Priority Programmes are characterized by their enhanced quality of research through the use of new methods and forms of collaboration in emerging fields, by added value through interdisciplinary cooperation, and by networking. The aim of the Priority Programme 1133 'Ultrafast Magnetization Processes' may be well characterized by the call for projects in June 2001 after the programme was approved by the Deutsche Forschungsgemeinschaft: 'The aim of the priority programme is the achievement of a basic understanding of the temporal evolution of fast magnetization processes in magnetically ordered films, multilayers and micro-structured systems. The challenge lies in the advancement of the field of ultrafast magnetization processes into the regime of a few femtoseconds to nanoseconds, a topic not yet well explored. A general aim is to understand the fundamental mechanisms needed for applications in ultrafast magneto-electronic devices. The fundamental topic to be addressed is the response of the magnetization of small structures upon the application of pulsed magnetic fields, laser pulses or injected spin-polarized electron pulses on short time scales, ranging from a small disturbance of the system up to the reversal of the magnetization direction.' Now, seven years later, the subject of ultrafast magnetization processes has grown into a mainstream research direction in modern magnetism. The major international conferences on magnetism, such as the Annual Conference on Magnetism and Magnetic Materials (MMM), the INTERMAG, the International Conference of Magnetism, as well as many regional conferences, schedule dedicated sessions to ultrafast magnetization processes, very often several of them. The large share in research in this field from German scientists has been made possible by this Priority Programme. Since its beginning, new developments have been picked up by the Priority Programme 1133 and addressed by projects. Spin torque phenomena in spin dynamics, although foreseen at the time of establishing the Priority Programme, have been taken up. The field of dissipation has been addressed and extended by several groups, with contributions both from theoretical and experimental groups. A first set of contributions addresses ultrafast dynamics and materials. T Roth et al [article 164001] in this issue] study the dynamics of coercivity in ultrafast pump-probe experiments on the femtosecond time scale. They show that an all optical pump-probe technique is, in general, not suitable for gaining access to the time-dependent behaviour of the coercivity, since the switching in a fixed external field is an irreversible process. They comment on the possible mechanisms leading to the observed reduction of the coercivity with increasing pump power and propose a potential solution to clarify the origin of such a behaviour. B Heitkamp et al [164002] discuss the femtosecond spin dynamics of ferromagnetic CoPt thin films and nanodots, which they probe using spin-polarized photoemission electron microscopy. They show by photoelectron spin analysis, that enhanced optical near 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 set of contributions addresses the field of spin waves and dynamic spin torque phenomena. C W Sandweg et al [164008] discuss the modification of the thermal spin wave spectrum by a domain wall in a narrow stripe and report the observation of a localized mode near the domain wall using the new technique of Brillouin light scattering microscopy. Time-resolved measurements are often made using a stroboscopic approach, thus missing non-periodic responses. P Möhrke et al [164009] report single-shot Kerr magnetometer measurements to observe the real time-domain wall motion in permalloy nanowires. The dynamics in magnetic disks is studied by I Neudecker et al [164010] using in-plane magnetic microwave fields for excitation. The effect of current-induced magnetization dynamics in single and double layer magnetic nanopillars is reported by N Müsgens et al [164011]. A spin-polarized charge current can modify the damping properties of spin waves in magnetic nanostructures. This is reported by V E Demidov et al [164012] using space-resolved Brillouin light scattering. They also present results regarding nonlinear spin-wave propagation and mode coupling in magnetic stripes and squares. D V Berkov and N L Gorn [164013] report on their results of nonlinear magnetization dynamics in nanodevices induced by a spin-polarized current using micromagnetic simulation. A third set of contributions focuses on dissipation phenomena ranging from a phenomenological description to the investigation of the microscopic origin(s). In a theory paper, M Fähnle et al [164014] revisit the Gilbert equation and discuss anisotropic and non-local damping of the magnetization dynamics. They derive their results by a combination of the breathing Fermi surface model with a variant of the ab initio density functional electron theory given by the magnetic force theorem. On the experimental side, S Serrano-Guisan et al [164015] address Gilbert damping in Ni81Fe19 thin films and microstructures using anisotropic magnetoresistance and pulsed inductive microwave magnetometry to measure the time-resolved precessional magnetization dynamics. The intrinsic and non-local Gilbert damping in polycrystalline Ni films is also addressed by J Walowski et al [164016] using femtosecond laser pulses. Several spin-wave modes are observed and their dissipation is studied. Non-local damping by spin currents emitted into a non-magnetic metallic layer of either vanadium, palladium or dysprosium is studied. Dissipation in small magnetic Ni81Fe19 rings is studied using Brillouin light scattering microscopy by H Schultheiss et al [164017]. They investigate the spatial profiles and the decay constants of spin-wave quasi-eigenmodes. We hope that this cluster of papers will help to stimulate and advance a better understanding of this very interesting field of ultrafast magnetization processes.

Nonequilibrium dynamics of the phonon gas in ultrafast-excited antimony

NASA Astrophysics Data System (ADS)

Krylow, Sergej; Zijlstra, Eeuwe S.; Kabeer, Fairoja Cheenicode; Zier, Tobias; Bauerhenne, Bernd; Garcia, Martin E.

2017-12-01

The ultrafast relaxation dynamics of a nonequilibrium phonon gas towards thermal equilibrium involves many-body collisions that cannot be properly described by perturbative approaches. Here, we develop a nonperturbative method to elucidate the microscopic mechanisms underlying the decay of laser-excited coherent phonons in the presence of electron-hole pairs, which so far are not fully understood. Our theory relies on ab initio molecular dynamics simulations on laser-excited potential-energy surfaces. Those simulations are compared with runs in which the laser-excited coherent phonon is artificially deoccupied. We apply this method to antimony and show that the decay of the A1 g phonon mode at low laser fluences can be accounted mainly to three-body down-conversion processes of an A1 g phonon into acoustic phonons. For higher excitation strengths, however, we see a crossover to a four-phonon process, in which two A1 g phonons decay into two optical phonons.

Tuning the nonlinear response of (6,5)-enriched single-wall carbon nanotubes dispersions

NASA Astrophysics Data System (ADS)

Aréstegui, O. S.; Silva, E. C. O.; Baggio, A. L.; Gontijo, R. N.; Hickmann, J. M.; Fantini, C.; Alencar, M. A. R. C.; Fonseca, E. J. S.

2017-04-01

Ultrafast nonlinear optical properties of (6,5)-enriched single-wall carbon nanotubes (SWCNTs) dispersions are investigated using the thermally managed Z-scan technique. As the (6,5) SWCNTs presented a strong resonance in the range of 895-1048 nm, the nonlinear refractive index (n2) and the absorption coefficients (β) measurements were performed tuning the laser exactly around absorption peak of the (6,5) SWCNTs. It is observed that the nonlinear response is very sensitive to the wavelength and the spectral behavior of n2 is strongly correlated to the tubes one-photon absorption band, presenting also a peak when the laser photon energy is near the tube resonance energy. This result suggests that a suitable selection of nanotubes types may provide optimized nonlinear optical responses in distinct regions of the electromagnetic spectrum. Analysis of the figures of merit indicated that this material is promising for ultrafast nonlinear optical applications under near infrared excitation.

How to manipulate magnetic states of antiferromagnets

NASA Astrophysics Data System (ADS)

Song, Cheng; You, Yunfeng; Chen, Xianzhe; Zhou, Xiaofeng; Wang, Yuyan; Pan, Feng

2018-03-01

Antiferromagnetic materials, which have drawn considerable attention recently, have fascinating features: they are robust against perturbation, produce no stray fields, and exhibit ultrafast dynamics. Discerning how to efficiently manipulate the magnetic state of an antiferromagnet is key to the development of antiferromagnetic spintronics. In this review, we introduce four main methods (magnetic, strain, electrical, and optical) to mediate the magnetic states and elaborate on intrinsic origins of different antiferromagnetic materials. Magnetic control includes a strong magnetic field, exchange bias, and field cooling, which are traditional and basic. Strain control involves the magnetic anisotropy effect or metamagnetic transition. Electrical control can be divided into two parts, electric field and electric current, both of which are convenient for practical applications. Optical control includes thermal and electronic excitation, an inertia-driven mechanism, and terahertz laser control, with the potential for ultrafast antiferromagnetic manipulation. This review sheds light on effective usage of antiferromagnets and provides a new perspective on antiferromagnetic spintronics.

Surface Plasmon-Mediated Nanoscale Localization of Laser-Driven sub-Terahertz Spin Dynamics in Magnetic Dielectrics

NASA Astrophysics Data System (ADS)

Chekhov, Alexander L.; Stognij, Alexander I.; Satoh, Takuya; Murzina, Tatiana V.; Razdolski, Ilya; Stupakiewicz, Andrzej

2018-05-01

Ultrafast all-optical control of spins with femtosecond laser pulses is one of the hot topics at the crossroads of photonics and magnetism with a direct impact on future magnetic recording. Unveiling light-assisted recording mechanisms for an increase of the bit density beyond the diffraction limit without excessive heating of the recording medium is an open challenge. Here we show that surface plasmon-polaritons in hybrid metal-dielectric structures can provide spatial confinement of the inverse Faraday effect, mediating the excitation of localized coherent spin precession with 0.41 THz frequency. We demonstrate a two orders of magnitude enhancement of the excitation efficiency at the surface plasmon resonance within the 100 nm layer in dielectric garnet. Our findings broaden the horizons of ultrafast spin-plasmonics and open pathways towards non-thermal opto-magnetic recording at the nano-scale.

Carrier-Specific Femtosecond XUV Transient Absorption of PbI 2 Reveals Ultrafast Nonradiative Recombination

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

Lin, Ming-Fu; Verkamp, Max A.; Leveillee, Joshua

Femtosecond carrier recombination in PbI 2 is measured using tabletop high-harmonic extreme ultraviolet (XUV) transient absorption spectroscopy and ultrafast electron diffraction. XUV absorption from 45 eV to 62 eV measures transitions from the iodine 4d core level to the conduction band density of states. Photoexcitation at 400 nm creates separate and distinct transient absorption signals for holes and electrons, separated in energy by the 2.4 eV band gap of the semiconductor. The shape of the conduction band and therefore the XUV absorption spectrum is temperature dependent, and nonradiative recombination converts the initial electronic excitation to thermal excitation within picoseconds. Ultrafastmore » electron diffraction (UED) is used to measure the lattice temperature and confirm the recombination mechanism. Lastly, the XUV and UED results support a 2nd-order recombination model with a rate constant of 2.5x10 -9 cm 3/s.« less

Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy

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

Guo, Zhi; Wan, Yan; Yang, Mengjin

The Shockley-Queisser limit for solar cell efficiency can be overcome if hot carriers can be harvested before they thermalize. Recently, carrier cooling time up to 100 picoseconds was observed in hybrid perovskites, but it is unclear whether these long-lived hot carriers can migrate long distance for efficient collection. Here, we report direct visualization of hot-carrier migration in methylammonium lead iodide (CH 3NH 3PbI 3) thin films by ultrafast transient absorption microscopy, demonstrating three distinct transport regimes. Quasiballistic transport was observed to correlate with excess kinetic energy, resulting in up to 230 nanometers transport distance that could overcome grain boundaries. Themore » nonequilibrium transport persisted over tens of picoseconds and ~600 nanometers before reaching the diffusive transport limit. Lastly, these results suggest potential applications of hot-carrier devices based on hybrid perovskites.« less

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.

Carrier-Specific Femtosecond XUV Transient Absorption of PbI 2 Reveals Ultrafast Nonradiative Recombination

DOE PAGES

Lin, Ming-Fu; Verkamp, Max A.; Leveillee, Joshua; ...

2017-11-30

Femtosecond carrier recombination in PbI 2 is measured using tabletop high-harmonic extreme ultraviolet (XUV) transient absorption spectroscopy and ultrafast electron diffraction. XUV absorption from 45 eV to 62 eV measures transitions from the iodine 4d core level to the conduction band density of states. Photoexcitation at 400 nm creates separate and distinct transient absorption signals for holes and electrons, separated in energy by the 2.4 eV band gap of the semiconductor. The shape of the conduction band and therefore the XUV absorption spectrum is temperature dependent, and nonradiative recombination converts the initial electronic excitation to thermal excitation within picoseconds. Ultrafastmore » electron diffraction (UED) is used to measure the lattice temperature and confirm the recombination mechanism. Lastly, the XUV and UED results support a 2nd-order recombination model with a rate constant of 2.5x10 -9 cm 3/s.« less

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.

Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy

DOE PAGES

Guo, Zhi; Wan, Yan; Yang, Mengjin; ...

2017-04-07

The Shockley-Queisser limit for solar cell efficiency can be overcome if hot carriers can be harvested before they thermalize. Recently, carrier cooling time up to 100 picoseconds was observed in hybrid perovskites, but it is unclear whether these long-lived hot carriers can migrate long distance for efficient collection. Here, we report direct visualization of hot-carrier migration in methylammonium lead iodide (CH 3NH 3PbI 3) thin films by ultrafast transient absorption microscopy, demonstrating three distinct transport regimes. Quasiballistic transport was observed to correlate with excess kinetic energy, resulting in up to 230 nanometers transport distance that could overcome grain boundaries. Themore » nonequilibrium transport persisted over tens of picoseconds and ~600 nanometers before reaching the diffusive transport limit. Lastly, these results suggest potential applications of hot-carrier devices based on hybrid perovskites.« less

Fast and high resolution thermal detector based on an aluminum nitride piezoelectric microelectromechanical resonator with an integrated suspended heat absorbing element

NASA Astrophysics Data System (ADS)

Hui, Yu; Rinaldi, Matteo

2013-03-01

This letter presents a miniaturized, fast, and high resolution thermal detector, in which a heat absorbing element and a temperature sensitive microelectromechanical system (MEMS) resonator are perfectly overlapped but separated by a microscale air gap. This unique design guarantees efficient and fast (˜10s μs) heat transfer from the absorbing element to the temperature sensitive device and enables high resolution thermal power detection (˜nW), thanks to the low noise performance of the high quality factor (Q = 2305) MEMS resonant thermal detector. A device prototype was fabricated, and its detection capabilities were experimentally characterized. A thermal power as low as 150 nW was experimentally measured, and a noise equivalent power of 6.5 nW/Hz1/2 was extracted. A device thermal time constant of only 350 μs was measured (smallest ever reported for MEMS resonant thermal detectors), indicating the great potential of the proposed technology for the implementation of ultra-fast and high resolution un-cooled resonant thermal detectors.

Directing the path of light-induced electron transfer at a molecular fork using vibrational excitation

NASA Astrophysics Data System (ADS)

Delor, Milan; Archer, Stuart A.; Keane, Theo; Meijer, Anthony J. H. M.; Sazanovich, Igor V.; Greetham, Gregory M.; Towrie, Michael; Weinstein, Julia A.

2017-11-01

Ultrafast electron transfer in condensed-phase molecular systems is often strongly coupled to intramolecular vibrations that can promote, suppress and direct electronic processes. Recent experiments exploring this phenomenon proved that light-induced electron transfer can be strongly modulated by vibrational excitation, suggesting a new avenue for active control over molecular function. Here, we achieve the first example of such explicit vibrational control through judicious design of a Pt(II)-acetylide charge-transfer donor-bridge-acceptor-bridge-donor 'fork' system: asymmetric 13C isotopic labelling of one of the two -C≡C- bridges makes the two parallel and otherwise identical donor→acceptor electron-transfer pathways structurally distinct, enabling independent vibrational perturbation of either. Applying an ultrafast UVpump(excitation)-IRpump(perturbation)-IRprobe(monitoring) pulse sequence, we show that the pathway that is vibrationally perturbed during UV-induced electron transfer is dramatically slowed down compared to its unperturbed counterpart. One can thus choose the dominant electron transfer pathway. The findings deliver a new opportunity for precise perturbative control of electronic energy propagation in molecular devices.

Ultrafast Coulomb-Induced Intervalley Coupling in Atomically Thin WS2.

PubMed

Schmidt, Robert; Berghäuser, Gunnar; Schneider, Robert; Selig, Malte; Tonndorf, Philipp; Malić, Ermin; Knorr, Andreas; Michaelis de Vasconcellos, Steffen; Bratschitsch, Rudolf

2016-05-11

Monolayers of semiconducting transition metal dichalcogenides hold the promise for a new paradigm in electronics by exploiting the valley degree of freedom in addition to charge and spin. For MoS2, WS2, and WSe2, valley polarization can be conveniently initialized and read out by circularly polarized light. However, the underlying microscopic processes governing valley polarization in these atomically thin equivalents of graphene are still not fully understood. Here, we present a joint experiment-theory study on the ultrafast time-resolved intervalley dynamics in monolayer WS2. Based on a microscopic theory, we reveal the many-particle mechanisms behind the observed spectral features. We show that Coulomb-induced intervalley coupling explains the immediate and prominent pump-probe signal in the unpumped valley and the seemingly low valley polarization degrees typically observed in pump-probe measurements compared to photoluminescence studies. The gained insights are also applicable to other light-emitting monolayer transition metal dichalcogenides, such as MoS2 and WSe2, where the Coulomb-induced intervalley coupling also determines the initial carrier dynamics.

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.

Ultrafast Screening and Quantitation of Pesticides in Food and Environmental Matrices by Solid-Phase Microextraction-Transmission Mode (SPME-TM) and Direct Analysis in Real Time (DART).

PubMed

Gómez-Ríos, Germán Augusto; Gionfriddo, Emanuela; Poole, Justen; Pawliszyn, Janusz

2017-07-05

The direct interface of microextraction technologies to mass spectrometry (MS) has unquestionably revolutionized the speed and efficacy at which complex matrices are analyzed. Solid Phase Micro Extraction-Transmission Mode (SPME-TM) is a technology conceived as an effective synergy between sample preparation and ambient ionization. Succinctly, the device consists of a mesh coated with polymeric particles that extracts analytes of interest present in a given sample matrix. This coated mesh acts as a transmission-mode substrate for Direct Analysis in Real Time (DART), allowing for rapid and efficient thermal desorption/ionization of analytes previously concentrated on the coating, and dramatically lowering the limits of detection attained by sole DART analysis. In this study, we present SPME-TM as a novel tool for the ultrafast enrichment of pesticides present in food and environmental matrices and their quantitative determination by MS via DART ionization. Limits of quantitation in the subnanogram per milliliter range can be attained, while total analysis time does not exceed 2 min per sample. In addition to target information obtained via tandem MS, retrospective studies of the same sample via high-resolution mass spectrometry (HRMS) were accomplished by thermally desorbing a different segment of the microextraction device.

Femtosecond laser polishing of optical materials

NASA Astrophysics Data System (ADS)

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

2015-10-01

Technologies including magnetorheological finishing and CNC polishing are commonly used to finish optical elements, but these methods are often expensive, generate waste through the use of fluids or abrasives, and may not be suited for specific freeform substrates due to the size and shape of finishing tools. Pulsed laser polishing has been demonstrated as a technique capable of achieving nanoscale roughness while offering waste-free fabrication, material-specific processing through direct tuning of laser radiation, and access to freeform shapes using refined beam delivery and focusing techniques. Nanosecond and microsecond pulse duration radiation has been used to perform successful melting-based polishing of a variety of different materials, but this approach leads to extensive heat accumulation resulting in subsurface damage. We have experimentally investigated the ability of femtosecond laser radiation to ablate silicon carbide and silicon. By substituting ultrafast laser radiation, polishing can be performed by direct evaporation of unwanted surface asperities with minimal heating and melting, potentially offering damage-free finishing of materials. Under unoptimized laser processing conditions, thermal effects can occur leading to material oxidation. To investigate these thermal effects, simulation of the heat accumulation mechanism in ultrafast laser ablation was performed. Simulations have been extended to investigate the optimum scanning speed and pulse energy required for processing various substrates. Modeling methodologies and simulation results will be presented.

Ablation-cooled material removal with ultrafast bursts of pulses

NASA Astrophysics Data System (ADS)

Kerse, Can; Kalaycıoğlu, Hamit; Elahi, Parviz; Çetin, Barbaros; Kesim, Denizhan K.; Akçaalan, Önder; Yavaş, Seydi; Aşık, Mehmet D.; Öktem, Bülent; Hoogland, Heinar; Holzwarth, Ronald; Ilday, Fatih Ömer

2016-09-01

The use of femtosecond laser pulses allows precise and thermal-damage-free removal of material (ablation) with wide-ranging scientific, medical and industrial applications. However, its potential is limited by the low speeds at which material can be removed and the complexity of the associated laser technology. The complexity of the laser design arises from the need to overcome the high pulse energy threshold for efficient ablation. However, the use of more powerful lasers to increase the ablation rate results in unwanted effects such as shielding, saturation and collateral damage from heat accumulation at higher laser powers. Here we circumvent this limitation by exploiting ablation cooling, in analogy to a technique routinely used in aerospace engineering. We apply ultrafast successions (bursts) of laser pulses to ablate the target material before the residual heat deposited by previous pulses diffuses away from the processing region. Proof-of-principle experiments on various substrates demonstrate that extremely high repetition rates, which make ablation cooling possible, reduce the laser pulse energies needed for ablation and increase the efficiency of the removal process by an order of magnitude over previously used laser parameters. We also demonstrate the removal of brain tissue at two cubic millimetres per minute and dentine at three cubic millimetres per minute without any thermal damage to the bulk.

Ablation-cooled material removal with ultrafast bursts of pulses.

PubMed

Kerse, Can; Kalaycıoğlu, Hamit; Elahi, Parviz; Çetin, Barbaros; Kesim, Denizhan K; Akçaalan, Önder; Yavaş, Seydi; Aşık, Mehmet D; Öktem, Bülent; Hoogland, Heinar; Holzwarth, Ronald; Ilday, Fatih Ömer

2016-09-01

The use of femtosecond laser pulses allows precise and thermal-damage-free removal of material (ablation) with wide-ranging scientific, medical and industrial applications. However, its potential is limited by the low speeds at which material can be removed and the complexity of the associated laser technology. The complexity of the laser design arises from the need to overcome the high pulse energy threshold for efficient ablation. However, the use of more powerful lasers to increase the ablation rate results in unwanted effects such as shielding, saturation and collateral damage from heat accumulation at higher laser powers. Here we circumvent this limitation by exploiting ablation cooling, in analogy to a technique routinely used in aerospace engineering. We apply ultrafast successions (bursts) of laser pulses to ablate the target material before the residual heat deposited by previous pulses diffuses away from the processing region. Proof-of-principle experiments on various substrates demonstrate that extremely high repetition rates, which make ablation cooling possible, reduce the laser pulse energies needed for ablation and increase the efficiency of the removal process by an order of magnitude over previously used laser parameters. We also demonstrate the removal of brain tissue at two cubic millimetres per minute and dentine at three cubic millimetres per minute without any thermal damage to the bulk.

Exploring the limits of ultrafast polymerase chain reaction using liquid for thermal heat exchange: A proof of principle

NASA Astrophysics Data System (ADS)

Maltezos, George; Johnston, Matthew; Taganov, Konstantin; Srichantaratsamee, Chutatip; Gorman, John; Baltimore, David; Chantratita, Wasun; Scherer, Axel

2010-12-01

Thermal ramp rate is a major limiting factor in using real-time polymerase chain reaction (PCR) for routine diagnostics. We explored the limits of speed by using liquid for thermal exchange rather than metal as in traditional devices, and by testing different polymerases. In a clinical setting, our system equaled or surpassed state-of-the-art devices for accuracy in amplifying DNA/RNA of avian influenza, cytomegalovirus, and human immunodeficiency virus. Using Thermococcus kodakaraensis polymerase and optimizing both electrical and chemical systems, we obtained an accurate, 35 cycle amplification of an 85-base pair fragment of E. coli O157:H7 Shiga toxin gene in as little as 94.1 s, a significant improvement over a typical 1 h PCR amplification.

Post-processing of 3D-printed parts using femtosecond and picosecond laser radiation

NASA Astrophysics Data System (ADS)

Mingareev, Ilya; Gehlich, Nils; Bonhoff, Tobias; Meiners, Wilhelm; Kelbassa, Ingomar; Biermann, Tim; Richardson, Martin C.

2014-03-01

Additive manufacturing, also known as 3D-printing, is a near-net shape manufacturing approach, delivering part geometry that can be considerably affected by various process conditions, heat-induced distortions, solidified melt droplets, partially fused powders, and surface modifications induced by the manufacturing tool motion and processing strategy. High-repetition rate femtosecond and picosecond laser radiation was utilized to improve surface quality of metal parts manufactured by laser additive techniques. Different laser scanning approaches were utilized to increase the ablation efficiency and to reduce the surface roughness while preserving the initial part geometry. We studied post-processing of 3D-shaped parts made of Nickel- and Titanium-base alloys by utilizing Selective Laser Melting (SLM) and Laser Metal Deposition (LMD) as additive manufacturing techniques. Process parameters such as the pulse energy, the number of layers and their spatial separation were varied. Surface processing in several layers was necessary to remove the excessive material, such as individual powder particles, and to reduce the average surface roughness from asdeposited 22-45 μm to a few microns. Due to the ultrafast laser-processing regime and the small heat-affected zone induced in materials, this novel integrated manufacturing approach can be used to post-process parts made of thermally and mechanically sensitive materials, and to attain complex designed shapes with micrometer precision.

Letters: Noise Equalization for Ultrafast Plane Wave Microvessel Imaging

PubMed Central

Song, Pengfei; Manduca, Armando; Trzasko, Joshua D.

2017-01-01

Ultrafast plane wave microvessel imaging significantly improves ultrasound Doppler sensitivity by increasing the number of Doppler ensembles that can be collected within a short period of time. The rich spatiotemporal plane wave data also enables more robust clutter filtering based on singular value decomposition (SVD). However, due to the lack of transmit focusing, plane wave microvessel imaging is very susceptible to noise. This study was designed to: 1) study the relationship between ultrasound system noise (primarily time gain compensation-induced) and microvessel blood flow signal; 2) propose an adaptive and computationally cost-effective noise equalization method that is independent of hardware or software imaging settings to improve microvessel image quality. PMID:28880169

Momentum space view of the ultrafast dynamics of surface photocurrents on topological insulators

NASA Astrophysics Data System (ADS)

Kuroda, K.; Reimann, J.; Güdde, J.; Höfer, U.

2017-02-01

The Dirac-cone surface states of topological insulators are characterized by a chiral spin texture in k-space with the electron spin locked to its parallel momentum. Mid-infrared pump pulses can induce spin-polarized photocurrents in such a topological surface state by optical transitions between the occupied and unoccupied part of the Dirac cone. We monitor the ultrafast dynamics of the corresponding asymmetric electron population in momentum space directly by time- and angle-resolved two-photon photoemission (2PPE). The elastic scattering times of 2.5 ps deduced for Sb2Te3 corresponds to a mean-fee path of 0.75 μm in real space.

Ultrafast Scavenging of the Precursor of H(•) Atom, (e(-), H3O(+)), in Aqueous Solutions.

PubMed

Balcerzyk, Anna; Schmidhammer, Uli; Wang, Furong; de la Lande, Aurélien; Mostafavi, Mehran

2016-09-01

Picosecond pulse radiolysis measurements have been performed in several highly concentrated HClO4 and H3PO4 aqueous solutions containing silver ions at different concentrations. Silver ion reduction is used to unravel the ultrafast reduction reactions observed at the end of a 7 ps electron pulse. Solvated electrons and silver atoms are observed by the pulse (electron beam)-probe (supercontinuum light) method. In highly acidic solutions, ultrafast reduction of silver ions is observed, a finding that is not compatible with a reaction between the H(•) atom and silver ions, which is known to be thermally activated. In addition, silver ion reduction is found to be even more efficient in phosphoric acid solution than that in neutral solution. In the acidic solutions investigated here, the species responsible for the reduction of silver atoms is considered to be the precursor of the H(•) atom. This precursor, denoted (e(-), H3O(+)), is a pair constituting an electron (not fully solvated) and H3O(+). Its structure differs from that of the pair of a solvated electron and a hydronium ion (es(-), H3O(+)), which absorbs in the visible region. The (e(-), H3O(+)) pair , called the pre-H(•) atom here, undergoes ultrafast electron transfer and can, like the presolvated electron, reduce silver ions much faster than the H(•) atom. Moreover, it is found that with the same concentration of H3O(+) the reduction reaction is favored in the phosphoric acid solution compared to that in the perchloric acid solution because of the less-efficient electron solvation process. The kinetics show that among the three reducing species, (e(-), H3O(+)), (es(-), H3O(+)), and H(•) atom, the first one is the most efficient.

Ultrafast excited-state dynamics in shape- and composition-controlled gold–silver bimetallic nanostructures

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

Zarick, Holly F.; Boulesbaa, Abdelaziz; Talbert, Eric M.

In this paper, we have examined the ultrafast dynamics of shape- and composition-controlled bimetallic Au/Ag core/shell nanostructures with transient absorption spectroscopy (TAS) as a function of Ag layer thickness (0–15 nm) and pump excitation fluence (50–500 nJ/pulse). Our synthesis approach generated both bimetallic nanocubes and nanopyramids with distinct dipolar plasmon resonances and plasmon dephasing behavior at the resonance. Lifetimes obtained from TAS at low powers (50 nJ/pulse) demonstrated minimal dependence on the Ag layer thickness, whereas at high power (500 nJ/pulse) a rise in electron–phonon coupling lifetime (τ 1) was observed with increasing Ag shell thickness for both nanocubes andmore » nanopyramids. This is attributable to the stronger absorption of the 400 nm pump pulse with higher Ag content, which induced higher electron temperatures. The phonon–phonon scattering lifetime (τ 2) also rises with increasing Ag layer, contributed both by the increasing size of the Au/Ag nanostructures as well as by surface chemistry effects. Further, we observed that even the thinnest, 2 nm, Ag shell strongly impacts both τ 1 and τ 2 at high power despite minimal change in overall size, indicating that the nanostructure composition also strongly impacts the thermalization temperature following absorption of 400 nm light. We also observed a shape-dependent trend at high power, where τ 2 increased for the nanopyramids with increasing Ag shell thickness and nanostructure size, but bimetallic nanocubes demonstrated an unexpected decrease in τ 2 for the thickest, 15 nm, Ag shell. This was attributed to the larger number of corners and edges in the nanocubes relative to the nanopyramids.« less

Ultrafast carrier dynamics in organic molecular crystals and conjugated polymers

NASA Astrophysics Data System (ADS)

Hegmann, Frank

2005-03-01

Organic semiconductors are being extensively studied by many research groups around the world for applications in electronic and photonic devices. For example, much work has focused on the development of organic thin film transistors based on thermally evaporated pentacene films, where the polycrystalline morphology typically results in a thermally-activated carrier mobility. On the other hand, more intrinsic bandlike transport, where the carrier mobility increases as the temperature decreases, has been observed in many organic single crystals. However, the nature of charge transport in organic molecular crystals is still not understood. Also, despite many advances in organic photonics, the nature of photocarrier generation in organic semiconductors is not completely understood and remains controversial even today. The generation of mobile charge carriers in photoexcited organic materials occurs over femtosecond to picosecond time scales, and so ultrafast pump-probe experiments are essential in order to improve our understanding of fundamental processes in these materials. Recently, time-resolved terahertz pulse spectroscopy has been used to directly probe transient photoconductivity in pentacene and functionalized pentacene thin films and single crystals [1,2], revealing photogeneration of mobile charge carriers over sub-picosecond time scales as well as bandlike carrier transport in both single crystal and thin film samples [1]. This talk will provide an overview of ultrafast carrier dynamics in organic semiconductors, and will emphasize how time-resolved terahertz pulse spectroscopy can be used to help understand the nature of photoexcitations and carrier transport in organic materials. (This work was supported by NSERC, CFI, CIPI, the Killam Trust, and ONR. Collaborators for this work are listed in Ref. 1.) [1] O. Ostroverkhova, D. G. Cooke, S. Shcherbyna, R. F. Egerton, F. A. Hegmann, R. R. Tykwinski, and J. E. Anthony, Phys. Rev. B., in press. [2] V. K. Thorsmølle, R. D. Averitt, X. Chi, D. J. Hilton, D. L. Smith, A. P. Ramirez, and A. J. Taylor, Appl. Phys. Lett. 84, 891 (2004).

Ultrafast Band Engineering and Transient Spin Currents in Antiferromagnetic Oxides

NASA Astrophysics Data System (ADS)

Gu, Mingqiang; Rondinelli, James M.

2016-04-01

We report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO3, we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observed in classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO3. These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices.

Ultrafast Band Engineering and Transient Spin Currents in Antiferromagnetic Oxides.

PubMed

Gu, Mingqiang; Rondinelli, James M

2016-04-29

We report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO3, we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observed in classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO3. These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices.

Ultrafast band engineering and transient spin currents in antiferromagnetic oxides

DOE PAGES

Gu, Mingqiang; Rondinelli, James M.

2016-04-29

Here, we report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO 3, we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observedmore » in classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO 3. These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices.« less

Ultrafast Band Engineering and Transient Spin Currents in Antiferromagnetic Oxides

PubMed Central

Gu, Mingqiang; Rondinelli, James M.

2016-01-01

We report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO3, we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observed in classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO3. These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices. PMID:27126354

Ultrafast laser-induced birefringence in various porosity silica glasses: from fused silica to aerogel.

PubMed

Cerkauskaite, Ausra; Drevinskas, Rokas; Rybaltovskii, Alexey O; Kazansky, Peter G

2017-04-03

We compare a femtosecond laser induced modification in silica matrices with three different degrees of porosity. In single pulse regime, the decrease of substrate density from fused silica to high-silica porous glass and to silica aerogel glass results in tenfold increase of laser affected region with the formation of a symmetric cavity surrounded by the compressed silica shell with pearl like structures. In multi-pulse regime, if the cavity produced by the first pulse is relatively large, the subsequent pulses do not cause further modifications. If not, the transition from void to the anisotropic structure with the optical axis oriented parallel to the incident polarization is observed. The maximum retardance value achieved in porous glass is twofold higher than in fused silica, and tenfold greater than in aerogel. The polarization sensitive structuring in porous glass by two pulses of ultrafast laser irradiation is demonstrated, as well as no observable stress is generated at any conditions.

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

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.

Depth-Dependent Defect Studies Using Coherent Acoustic Phonons

DTIC Science & Technology

2014-09-29

using CAP waves as an active moving interface to induce local changes in electric, acoustic , and optical properties. This is able to generate ultrafast...the elastic strain component [6]. b) Modification of the crystal lattice due to transient strain caused by the coherent acoustic phonon wave . The...opto-electronic properties of materials. We are also using CAP waves as an active moving interface to induce local changes in electric, acoustic , and

Ultrafast Laser Interaction Processes for Libs and Other Sensing Technologies

DTIC Science & Technology

2013-04-05

Wang. Propagation of ultrashort pulses through water, Optics Express, (02 2007): . doi: 12/02/2009 8.00 Z. Chen, S. Mao. Femtosecond laser -induced...Richardson, "Nd:YAG-CO2 double- pulse laser -induced breakdown spectroscopy for explosive residues detection" SPIE Defense, Security, Sensing; Orlando, FL... Ultrashort Pulse Laser Workshop, Directed Energy Professional Society; Newton, MA, USA; 06/29,2009. 63. Martin C. Richardson, Michael Sigman

Structural modifications induced in dentin by femtosecond laser

NASA Astrophysics Data System (ADS)

Le, Quang-Tri; Bertrand, Caroline; Vilar, Rui

2016-12-01

The structural and chemical modifications induced in dentin by ultrafast laser ablation were studied. The laser experiments were performed with a Yb:KYW chirped-pulse-regenerative amplification laser system (560-fs pulse duration, 1030-nm radiation wavelength), fluences in the range 2 to 14 J/cm2, 1-kHz pulse repetition rate, and 5-mm/s scanning speed. The ablation surfaces were characterized by scanning electron microscopy and Fourier transform infrared spectroscopy. The ablation surfaces produced with 2 J/cm2 presented an irregular morphology with exposed dentinal tubules and no evidence of thermal effects. For 7 and 14 J/cm2, the ablation surfaces were covered by a layer of redeposited ablation debris, consisting mainly of amorphous calcium phosphate. This layer is weakly adherent to the underlying tissue and can be easily removed by ultrasonication, revealing a surface with a morphology similar to the one obtained with 2 J/cm2. The constitution of the dentin ablation surfaces is similar to the constitution of pristine dentin, showing that, within this fluence range, the laser treatment does not significantly modify the structure and constitution of dentin. The results achieved suggest an ablation mechanism where collagen is preferentially decomposed by the laser radiation, reducing the tissue cohesive strength and leading, ultimately, to its ablation.

Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics

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

Kunnus, Kristjan; Josefsson, Ida; Rajkovic, Ivan

Here, ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbitalmore » and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)5 in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.« less

Phase diagram of the ultrafast photoinduced insulator-metal transition in vanadium dioxide

NASA Astrophysics Data System (ADS)

Cocker, T. L.; Titova, L. V.; Fourmaux, S.; Holloway, G.; Bandulet, H.-C.; Brassard, D.; Kieffer, J.-C.; El Khakani, M. A.; Hegmann, F. A.

2012-04-01

We use time-resolved terahertz spectroscopy to probe the ultrafast dynamics of the insulator-metal phase transition induced by femtosecond laser pulses in a nanogranular vanadium dioxide (VO2) film. Based on the observed thresholds for characteristic transient terahertz dynamics, a phase diagram of critical pump fluence versus temperature for the insulator-metal phase transition in VO2 is established for the first time over a broad range of temperatures down to 17 K. We find that both Mott and Peierls mechanisms are present in the insulating state and that the photoinduced transition is nonthermal. We propose a critical-threshold model for the ultrafast photoinduced transition based on a critical density of electrons and a critical density of coherently excited phonons necessary for the structural transition to the metallic state. As a result, evidence is found at low temperatures for an intermediate metallic state wherein the Mott state is melted but the Peierls distortion remains intact, consistent with recent theoretical predictions. Finally, the observed terahertz conductivity dynamics above the photoinduced transition threshold reveal nucleation and growth of metallic nanodomains over picosecond time scales.

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.

Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics

DOE PAGES

Kunnus, Kristjan; Josefsson, Ida; Rajkovic, Ivan; ...

2016-10-07

Here, ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbitalmore » and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)5 in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.« less

Tunable and switchable dual-waveband ultrafast fiber laser with 100 GHz repetition-rate.

PubMed

Tan, Xiao-Mei; Chen, Hong-Jie; Cui, Hu; Lv, Yao-Kun; Zhao, Guan-Kai; Luo, Zhi-Chao; Luo, Ai-Ping; Xu, Wen-Cheng

2017-07-10

We demonstrate a tunable and switchable dual-waveband 100 GHz high-repetition-rate (HRR) ultrafast fiber laser based on dissipative four-wave-mixing (DFWM) mode-locked technique. Each waveband maintains HRR operation. The DFWM effect was realized by combining a Fabry-Perot (F-P) filter and a piece of highly nonlinear fiber (HNLF). The tunable and switchable operations were achieved by nonlinear polarization rotation (NPR) technique. Through appropriately controlling the filtering effect induced by NPR, the laser could operate at two kinds of tunable regimes. One is that the spacing between these two wavebands could be tuned while keeping their center at 1559 nm. The other is that the central position of the entire dual-waveband is tunable while with the same separation between these two wavebands of 13.2 nm. Moreover, the laser could switch between these two wavebands. Correspondingly, the center of the single-waveband has a tuning range of 15.2 nm. This versatile ultrafast fiber laser may find applications in fields of optical frequency combs, high speed optical communications, where HRR pulses are necessary.

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

Interlayer‐State‐Coupling Dependent Ultrafast Charge Transfer in MoS2/WS2 Bilayers

PubMed Central

Zhang, Jin; Hong, Hao; Lian, Chao; Ma, Wei; Xu, Xiaozhi; Zhou, Xu; Fu, Huixia

2017-01-01

Light‐induced interlayer ultrafast charge transfer in 2D heterostructures provides a new platform for optoelectronic and photovoltaic applications. The charge separation process is generally hypothesized to be dependent on the interlayer stackings and interactions, however, the quantitative characteristic and detailed mechanism remain elusive. Here, a systematical study on the interlayer charge transfer in model MoS2/WS2 bilayer system with variable stacking configurations by time‐dependent density functional theory methods is demonstrated. The results show that the slight change of interlayer geometry can significantly modulate the charge transfer time from 100 fs to 1 ps scale. Detailed analysis further reveals that the transfer rate in MoS2/WS2 bilayers is governed by the electronic coupling between specific interlayer states, rather than the interlayer distances, and follows a universal dependence on the state‐coupling strength. The results establish the interlayer stacking as an effective freedom to control ultrafast charge transfer dynamics in 2D heterostructures and facilitate their future applications in optoelectronics and light harvesting. PMID:28932669

Ultrafast time scale X-rotation of cold atom storage qubit using Rubidium clock states

NASA Astrophysics Data System (ADS)

Song, Yunheung; Lee, Han-Gyeol; Kim, Hyosub; Jo, Hanlae; Ahn, Jaewook

2017-04-01

Ultrafast-time-scale optical interaction is a local operation on the electronic subspace of an atom, thus leaving its nuclear state intact. However, because atomic clock states are maximally entangled states of the electronic and nuclear degrees of freedom, their entire Hilbert space should be accessible only with local operations and classical communications (LOCC). Therefore, it may be possible to achieve hyperfine qubit gates only with electronic transitions. Here we show an experimental implementation of ultrafast X-rotation of atomic hyperfine qubits, in which an optical Rabi oscillation induces a geometric phase between the constituent fine-structure states, thus bringing about the X-rotation between the two ground hyperfine levels. In experiments, cold atoms in a magneto-optical trap were controlled with a femtosecond laser pulse from a Ti:sapphire laser amplifier. Absorption imaging of the as-controlled atoms initially in the ground hyperfine state manifested polarization dependence, strongly agreeing with the theory. The result indicates that single laser pulse implementations of THz clock speed qubit controls are feasible for atomic storage qubits. Samsung Science and Technology Foundation [SSTF-BA1301-12].

Ultrafast chemical interface scattering as an additional decay channel for nascent nonthermal electrons in small metal nanoparticles.

PubMed

Bauer, Christophe; Abid, Jean-Pierre; Fermin, David; Girault, Hubert H

2004-05-15

The use of 4.2 nm gold nanoparticles wrapped in an adsorbates shell and embedded in a TiO2 metal oxide matrix gives the opportunity to investigate ultrafast electron-electron scattering dynamics in combination with electronic surface phenomena via the surface plasmon lifetimes. These gold nanoparticles (NPs) exhibit a large nonclassical broadening of the surface plasmon band, which is attributed to a chemical interface damping. The acceleration of the loss of surface plasmon phase coherence indicates that the energy and the momentum of the collective electrons can be dissipated into electronic affinity levels of adsorbates. As a result of the preparation process, gold NPs are wrapped in a shell of sulfate compounds that gives rise to a large density of interfacial molecules confined between Au and TiO2, as revealed by Fourier-transform-infrared spectroscopy. A detailed analysis of the transient absorption spectra obtained by broadband femtosecond transient absorption spectroscopy allows separating electron-electron and electron-phonon interaction. Internal thermalization times (electron-electron scattering) are determined by probing the decay of nascent nonthermal electrons (NNEs) and the build-up of the Fermi-Dirac electron distribution, giving time constants of 540 to 760 fs at 0.42 and 0.34 eV from the Fermi level, respectively. Comparison with literature data reveals that lifetimes of NNEs measured for these small gold NPs are more than four times longer than for silver NPs with similar sizes. The surprisingly long internal thermalization time is attributed to an additional decay mechanism (besides the classical e-e scattering) for the energy loss of NNEs, identified as the ultrafast chemical interface scattering process. NNEs experience an inelastic resonant scattering process into unoccupied electronic states of adsorbates, that directly act as an efficient heat bath, via the excitation of molecular vibrational modes. The two-temperature model is no longer valid for this system because of (i) the temporal overlap between the internal and external thermalization process is very important; (ii) a part of the photonic energy is directly transferred toward the adsorbates (not among "cold" conduction band electrons). These findings have important consequence for femtochemistry on metal surfaces since they show that reactions can be initiated by nascent nonthermal electrons (as photoexcited, out of a Fermi-Dirac distribution) besides of the hot electron gas.

Modeling of silicon in femtosecond laser-induced modification regimes: accounting for ambipolar diffusion

NASA Astrophysics Data System (ADS)

Derrien, Thibault J.-Y.; Bulgakova, Nadezhda M.

2017-05-01

During the last decades, femtosecond laser irradiation of materials has led to the emergence of various applications based on functionalization of surfaces at the nano- and microscale. Via inducing a periodic modification on material surfaces (band gap modification, nanostructure formation, crystallization or amorphization), optical and mechanical properties can be tailored, thus turning femtosecond laser to a key technology for development of nanophotonics, bionanoengineering, and nanomechanics. Although modification of semiconductor surfaces with femtosecond laser pulses has been studied for more than two decades, the dynamics of coupling of intense laser light with excited matter remains incompletely understood. In particular, swift formation of a transient overdense electron-hole plasma dynamically modifies optical properties in the material surface layer and induces large gradients of hot charge carriers, resulting in ultrafast charge-transport phenomena. In this work, the dynamics of ultrafast laser excitation of a semiconductor material is studied theoretically on the example of silicon. A special attention is paid to the electron-hole pair dynamics, taking into account ambipolar diffusion effects. The results are compared with previously developed simulation models, and a discussion of the role of charge-carrier dynamics in localization of material modification is provided.

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.

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.

Slow Organic-to-Inorganic Sub-Lattice Thermalization in Methylammonium Lead Halide Perovskites Observed by Ultrafast Photoluminescence

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

Chang, Angela Y.; Cho, Yi-Ju; Chen, Kuan-Chen

2016-05-31

Carrier dynamics in methylammonium lead halide (CH3NH3PbI3-xClx) perovskite thin films, of differing crystal morphology, are examined as functions of temperature and excitation wavelength. At room temperature, long-lived (> nanosecond) transient absorption signals indicate negligible carrier trapping. However, in measurements of ultrafast photoluminescence excited at 400 nm, a heretofore unexplained, large amplitude (50%-60%), 45 ps decay process is observed. This feature persists for temperatures down to the orthorhombic phase transition. Varying pump photon energy reveals that the fast, band-edge photoluminescence (PL) decay only appears for excitation >= 2.38 eV (520 nm), with larger amplitudes for higher pump energies. Lower photon-energy excitationmore » yields slow dynamics consistent with negligible carrier trapping. Further, sub-bandgap two-photon pumping yields identical PL dynamics as direct absorption, signifying sensitivity to the total deposited energy and insensitivity to interfacial effects. Together with first principles electronic structure and ab initio molecular dynamics calculations, the results suggest the fast PL decay stems from excitation of high energy phonon modes associated with the organic sub-lattice that temporarily enhance wavefunction overlap within the inorganic component owing to atomic displacement, thereby transiently changing the PL radiative rate during thermalization. Hence, the fast PL decay relates a characteristic organic-to-inorganic sub-lattice equilibration timescale at optoelectronic-relevant excitation energies.« less

Ultrafast control of strong light-matter coupling

NASA Astrophysics Data System (ADS)

Lange, Christoph; Cancellieri, Emiliano; Panna, Dmitry; Whittaker, David M.; Steger, Mark; Snoke, David W.; Pfeiffer, Loren N.; West, Kenneth W.; Hayat, Alex

2018-01-01

We dynamically modulate strong light-matter coupling in a GaAs/AlGaAs microcavity using intense ultrashort laser pulses tuned below the interband exciton energy, which induce a transient Stark shift of the cavity polaritons. For 225-fs pulses, shorter than the cavity Rabi cycle period of 1000 fs, this shift decouples excitons and cavity photons for the duration of the pulse, interrupting the periodic energy exchange between photonic and electronic states. For 1500-fs pulses, longer than the Rabi cycle period, however, the Stark shift does not affect the strong coupling. The two regimes are marked by distinctly different line shapes in ultrafast reflectivity measurements—regardless of the Stark field intensity. The crossover marks the transition from adiabatic to diabatic switching of strong light-matter coupling.

Ultrafast spintronics roadmap: from femtosecond spin current pulses to terahertz non-uniform spin dynamics via nano-confined spin transfer torques (Conference Presentation)

NASA Astrophysics Data System (ADS)

Melnikov, Alexey; Razdolski, Ilya; Alekhin, Alexandr; Ilin, Nikita; Meyburg, Jan; Diesing, Detlef; Roddatis, Vladimir; Rungger, Ivan; Stamenova, Maria; Sanvito, Stefano; Bovensiepen, Uwe

2016-10-01

Further development of spintronics requires miniaturization and reduction of characteristic timescales of spin dynamics combining the nanometer spatial and femtosecond temporal ranges. These demands shift the focus of interest towards the fundamental open question of the interaction of femtosecond spin current (SC) pulses with a ferromagnet (FM). The spatio-temporal properties of the spin transfer torque (STT) exerted by ultrashort SC pulses on the FM open the time domain for studying STT fingerprint on spatially non-uniform magnetization dynamics. Using the sensitivity of magneto-induced second harmonic generation to SC, we develop technique for SC monitoring. With 20 fs resolution, we demonstrate the generation of 250 fs-long SC pulses in Fe/Au/Fe/MgO(001) structures. Their temporal profile indicates (i) nearly-ballistic hot electron transport in Au and (ii) that the pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Together with strongly spin-dependent Fe/Au interface transmission calculated for these carriers, this suggests the non-thermal spin-dependent Seebeck effect dominating the generation of ultrashort SC pulses. The analysis of SC transmission/reflection at the Au/Fe interface shows that hot electron spins orthogonal to the Fe magnetization rotate gaining huge parallel (anti-parallel) projection in transmitted (reflected) SC. This is accompanied by a STT-induced perturbation of the magnetization localized at the interface, which excites the inhomogeneous high-frequency spin dynamics in the FM. Time-resolved magneto-optical studies reveal the excitation of several standing spin wave modes in the Fe film with their spectrum extending up to 0.6 THz and indicating the STT spatial confinement to 2 nm.

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

Inhomogeneity of the ultrafast insulator-to-metal transition dynamics of VO2.

PubMed

O'Callahan, Brian T; Jones, Andrew C; Hyung Park, Jae; Cobden, David H; Atkin, Joanna M; Raschke, Markus B

2015-04-21

The insulator-metal transition (IMT) of vanadium dioxide (VO2) has remained a long-standing challenge in correlated electron physics since its discovery five decades ago. Most interpretations of experimental observations have implicitly assumed a homogeneous material response. Here we reveal inhomogeneous behaviour of even individual VO2 microcrystals using pump-probe microscopy and nanoimaging. The timescales of the ultrafast IMT vary from 40±8 fs, that is, shorter than a suggested phonon bottleneck, to 200±20 fs, uncorrelated with crystal size, transition temperature and initial insulating structural phase, with average value similar to results from polycrystalline thin-film studies. In combination with the observed sensitive variations in the thermal nanodomain IMT behaviour, this suggests that the IMT is highly susceptible to local changes in, for example, doping, defects and strain. Our results suggest an electronic mechanism dominating the photoinduced IMT, but also highlight the difficulty to deduce microscopic mechanisms when the true intrinsic material response is yet unclear.

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.

Ultra-fast DNA-based multiplex convection PCR method for meat species identification with possible on-site applications.

PubMed

Song, Kyung-Young; Hwang, Hyun Jin; Kim, Jeong Hee

2017-08-15

The aim of this study was to develop an ultra-fast molecular detection method for meat identification using convection Palm polymerase chain reaction (PCR). The mitochondrial cytochrome b (Cyt b) gene was used as a target gene. Amplicon size was designed to be different for beef, lamb, and pork. When these primer sets were used, each species-specific set specifically detected the target meat species in singleplex and multiplex modes in a 24min PCR run. The detection limit was 1pg of DNA for each meat species. The convection PCR method could detect as low as 1% of meat adulteration. The stability of the assay was confirmed using thermal processed meats. We also showed that direct PCR can be successfully performed with mixed meats and food samples. These results suggest that the developed assay may be useful in the authentication of meats and meat products in laboratory and rapid on-site applications. Copyright © 2017 Elsevier Ltd. All rights reserved.

Dynamics of liquids, molecules, and proteins measured with ultrafast 2D IR vibrational echo chemical exchange spectroscopy.

PubMed

Fayer, M D

2009-01-01

A wide variety of molecular systems undergo fast structural changes under thermal equilibrium conditions. Such transformations are involved in a vast array of chemical problems. Experimentally measuring equilibrium dynamics is a challenging problem that is at the forefront of chemical research. This review describes ultrafast 2D IR vibrational echo chemical exchange experiments and applies them to several types of molecular systems. The formation and dissociation of organic solute-solvent complexes are directly observed. The dissociation times of 13 complexes, ranging from 4 ps to 140 ps, are shown to obey a relationship that depends on the complex's formation enthalpy. The rate of rotational gauche-trans isomerization around a carbon-carbon single bond is determined for a substituted ethane at room temperature in a low viscosity solvent. The results are used to obtain an approximate isomerization rate for ethane. Finally, the time dependence of a well-defined single structural transformation of a protein is measured.

Optothermal response of a single silicon nanotip

NASA Astrophysics Data System (ADS)

Vella, A.; Shinde, D.; Houard, J.; Silaeva, E.; Arnoldi, L.; Blum, I.; Rigutti, L.; Pertreux, E.; Maioli, P.; Crut, A.; Del Fatti, N.

2018-02-01

The optical properties and thermal dynamics of conical single silicon nanotips are experimentally and theoretically investigated. The spectral and spatial dependencies of their optical extinction are quantitatively measured by spatial modulation spectroscopy (SMS). A nonuniform optical extinction along the tip axis and an enhanced near-infrared absorption, as compared to bulk crystalline silicon, are evidenced. This information is a key input for computing the thermal response of single silicon nanotips under ultrafast laser illumination, which is investigated by laser assisted atom probe tomography (La-APT) used as a highly sensitive temperature probe. A combination of these two experimental techniques and comparison with modeling also permits us to elucidate the impact of thermal effects on the laser assisted field evaporation process. Extension of this coupled approach opens up future perspectives for the quantitative study of the optical and thermal properties of a wide class of individual nano-objects, in particular elongated ones such as nanotubes, nanowires, and nanocones, which constitute promising nanosources for electron and/or ion emission.

Interband and intraband electron kinetics in non-thermal warm dense gold

NASA Astrophysics Data System (ADS)

Brennan Brown, Shaughnessy; Chen, Zhijiang; Curry, Chandra; Hering, Philippe; Hoffmann, Matthias C.; Ng, Andrew; Reid, Matthew; Tsui, Ying Y.; Glenzer, Siegfried H.

2015-11-01

Single-state warm dense matter may be produced via isochoric heating of thin metal foils using ultrafast high-power lasers. Previous experiments have confirmed that electron temperatures exceed ion temperatures during the initial picoseconds following excitation; however, electron kinetics in non-thermal states preceding establishment of a well-defined electron thermal distribution remain little understood. X-ray and optical probing techniques provide necessary resolution to investigate these electronic properties. Here, we will present a study of electron kinetics in warm dense gold produced by irradiating free-standing 30 nm Au foils with a 400 nm FWHM, 45 fs Ti:Sapphire laser system at SLAC National Accelerator Laboratory. The temporal evolutions of AC conductivity for 400 nm and 800 nm laser pulses are simultaneously determined with sub-100 fs resolution, providing insight into the 5 d-6 s/ p interband and 6 s / p intraband transitions respectively. Our results suggest that Auger decay and three-body recombination play important roles in electron thermalization of warm dense gold.

New opportunities at the frontiers of spintronics

DOE PAGES

Hoffmann, Axel; Bader, Sam D.

2015-10-05

The field of spintronics, or magnetic electronics, is maturing and giving rise to new subfields. These new directions involve the study of collective spin excitations and couplings of the spin system to additional degrees of freedom of a material, as well as metastable phenomena due to perturbations that drive the system far from equilibrium. The interactions lead to possibilities for future applications within the realm of energy-efficient information technologies. Examples discussed herein include research opportunities associated with (i) various spin-orbit couplings, such as spin Hall effects, (ii) couplings to the thermal bath of a system, such as in spin Seebeckmore » effects, (iii) spin-spin couplings, such as via induced and interacting magnon excitations, and (iv) spin-photon couplings, such as in ultra-fast magnetization switching due to coherent photon pulses. These four basic frontier areas of research are giving rise to new applied disciplines known as spin-orbitronics, spin-caloritronics, magnonics, and spin-photonics, respectively. These topics are highlighted in order to stimulate interest in the new directions that spintronics research is taking, and to identify open issues to pursue.« less

Effects of Carrier Confinement and Intervalley Scattering on Photoexcited Electron Plasma in Silicon.

PubMed

Sieradzki, A; Kuznicki, Z T

2013-01-01

The ultrafast reflectivity of silicon, excited and probed with femtosecond laser pulses, is studied for different wavelengths and energy densities. The confinement of carriers in a thin surface layer delimited by a nanoscale Si-layered system buried in a Si heavily-doped wafer reduces the critical density of carriers necessary to create the electron plasma by a factor of ten. We performed two types of reflectivity measurements, using either a single beam or two beams. The plasma strongly depends on the photon energy density because of the intervalley scattering of the electrons revealed by two different mechanisms assisted by the electron-phonon interaction. One mechanism leads to a negative differential reflectivity that can be attributed to an induced absorption in X valleys. The other mechanism occurs, when the carrier population is thermalizing and gives rise to a positive differential reflectivity corresponding to Pauli-blocked intervalley gamma to X scattering. These results are important for improving the efficiency of Si light-to-electricity converters, in which there is a possibility of multiplying carriers by nanostructurization of Si.

Control of terahertz nonlinear transmission with electrically gated graphene metadevices.

PubMed

Choi, Hyun Joo; Baek, In Hyung; Kang, Bong Joo; Kim, Hyeon-Don; Oh, Sang Soon; Hamm, Joachim M; Pusch, Andreas; Park, Jagang; Lee, Kanghee; Son, Jaehyeon; Jeong, Young U K; Hess, Ortwin; Rotermund, Fabian; Min, Bumki

2017-02-20

Graphene, which is a two-dimensional crystal of carbon atoms arranged in a hexagonal lattice, has attracted a great amount of attention due to its outstanding mechanical, thermal and electronic properties. Moreover, graphene shows an exceptionally strong tunable light-matter interaction that depends on the Fermi level - a function of chemical doping and external gate voltage - and the electromagnetic resonance provided by intentionally engineered structures. In the optical regime, the nonlinearities of graphene originated from the Pauli blocking have already been exploited for mode-locking device applications in ultrafast laser technology, whereas nonlinearities in the terahertz regime, which arise from a reduction in conductivity due to carrier heating, have only recently been confirmed experimentally. Here, we investigated two key factors for controlling nonlinear interactions of graphene with an intense terahertz field. The induced transparencies of graphene can be controlled effectively by engineering meta-atoms and/or changing the number of charge carriers through electrical gating. Additionally, nonlinear phase changes of the transmitted terahertz field can be observed by introducing the resonances of the meta-atoms.

Solid-State Explosive Reaction for Nanoporous Bulk Thermoelectric Materials.

PubMed

Zhao, Kunpeng; Duan, Haozhi; Raghavendra, Nunna; Qiu, Pengfei; Zeng, Yi; Zhang, Wenqing; Yang, Jihui; Shi, Xun; Chen, Lidong

2017-11-01

High-performance thermoelectric materials require ultralow lattice thermal conductivity typically through either shortening the phonon mean free path or reducing the specific heat. Beyond these two approaches, a new unique, simple, yet ultrafast solid-state explosive reaction is proposed to fabricate nanoporous bulk thermoelectric materials with well-controlled pore sizes and distributions to suppress thermal conductivity. By investigating a wide variety of functional materials, general criteria for solid-state explosive reactions are built upon both thermodynamics and kinetics, and then successfully used to tailor material's microstructures and porosity. A drastic decrease in lattice thermal conductivity down below the minimum value of the fully densified materials and enhancement in thermoelectric figure of merit are achieved in porous bulk materials. This work demonstrates that controlling materials' porosity is a very effective strategy and is easy to be combined with other approaches for optimizing thermoelectric performance. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Comparison of the ultrafast hot electron dynamics of titanium nitride and gold for plasmonic applications

NASA Astrophysics Data System (ADS)

Doiron, Brock; Li, Yi; Mihai, Andrei P.; Cohen, Lesley F.; Petrov, Peter K.; Alford, Neil M.; Oulton, Rupert F.; Maier, Stefan A.

2017-08-01

With similar optical properties to gold and high thermal stability, titanium nitride continues to prove itself as a promising plasmonic material for high-temperature applications in the visible and near-infrared. In this work, we use transient pump probe differential reflection measurements to compare the electron energy decay channels in titanium nitride and gold thin films. Using an extended two temperature model to incorporate the photoexcited electrons, it is possible to separate the electron-electron and electron-phonon scattering contributions immediately following the arrival of the pump pulse. This model allows for incredibly accurate determination of the internal electronic properties using only optical measurements. As the electronic properties are key in hot electron applications, we show that titanium nitide has substantially longer electron thermalization and electron-phonon scattering times. With this, we were also able to resolve electron thermal conduction in the film using purely optical measurements.

Direct observation of ultrafast-electron-transfer reactions unravels high effectiveness of reductive DNA damage

PubMed Central

Nguyen, Jenny; Ma, Yuhan; Luo, Ting; Bristow, Robert G.; Jaffray, David A.; Lu, Qing-Bin

2011-01-01

Both water and electron-transfer reactions play important roles in chemistry, physics, biology, and the environment. Oxidative DNA damage is a well-known mechanism, whereas the relative role of reductive DNA damage is unknown. The prehydrated electron (), a novel species of electrons in water, is a fascinating species due to its fundamental importance in chemistry, biology, and the environment. is an ideal agent to observe reductive DNA damage. Here, we report both the first in situ femtosecond time-resolved laser spectroscopy measurements of ultrafast-electron-transfer (UET) reactions of with various scavengers (KNO3, isopropanol, and dimethyl sulfoxide) and the first gel electrophoresis measurements of DNA strand breaks induced by and OH• radicals co-produced by two-UV-photon photolysis of water. We strikingly found that the yield of reductive DNA strand breaks induced by each is twice the yield of oxidative DNA strand breaks induced by each OH• radical. Our results not only unravel the long-standing mystery about the relative role of radicals in inducing DNA damage under ionizing radiation, but also challenge the conventional notion that oxidative damage is the main pathway for DNA damage. The results also show the potential of femtomedicine as a new transdisciplinary frontier and the broad significance of UET reactions of in many processes in chemistry, physics, biology, and the environment. PMID:21730183

Towards industrial ultrafast laser microwelding: SiO2 and BK7 to aluminum alloy.

PubMed

Carter, Richard M; Troughton, Michael; Chen, Jianyong; Elder, Ian; Thomson, Robert R; Daniel Esser, M J; Lamb, Robert A; Hand, Duncan P

2017-06-01

We report systematic analysis and comparison of ps-laser microwelding of industry relevant Al6082 parts to SiO 2 and BK7. Parameter mapping of pulse energy and focal depth on the weld strength is presented. The welding process was found to be strongly dependent on the focal plane but has a large tolerance to variation in pulse energy. Accelerated lifetime tests by thermal cycling from -50° to +90°C are presented. Welds in Al6082-BK7 parts survive over the full temperature range where the ratio of thermal expansion coefficients is 3.4:1. Welds in Al6082-SiO 2 parts (ratio 47.1:1) survive only a limited temperature range.

Ultrafast Flame Annealing of TiO2 Paste for Fabricating Dye-Sensitized and Perovskite Solar Cells with Enhanced Efficiency.

PubMed

Kim, Jung Kyu; Chai, Sung Uk; Cho, Yoonjun; Cai, Lili; Kim, Sung June; Park, Sangwook; Park, Jong Hyeok; Zheng, Xiaolin

2017-11-01

Mesoporous TiO 2 nanoparticle (NP) films are broadly used as electrodes in photoelectrochemical cells, dye-sensitized solar cells (DSSCs), and perovskite solar cells (PSCs). State-of-the-art mesoporous TiO 2 NP films for these solar cells are fabricated by annealing TiO 2 paste-coated fluorine-doped tin oxide glass in a box furnace at 500 °C for ≈30 min. Here, the use of a nontraditional reactor, i.e., flame, is reported for the high throughput and ultrafast annealing of TiO 2 paste (≈1 min). This flame-annealing method, compared to conventional furnace annealing, exhibits three distinct benefits. First, flame removes polymeric binders in the initial TiO 2 paste more completely because of its high temperature (≈1000 °C). Second, flame induces strong interconnections between TiO 2 nanoparticles without affecting the underlying transparent conducting oxide substrate. Third, the flame-induced carbothermic reduction on the TiO 2 surface facilitates charge injection from the dye/perovskite to TiO 2 . Consequently, when the flame-annealed mesoporous TiO 2 film is used to fabricate DSSCs and PSCs, both exhibit enhanced charge transport and higher power conversion efficiencies than those fabricated using furnace-annealed TiO 2 films. Finally, when the ultrafast flame-annealing method is combined with a fast dye-coating method to fabricate DSSC devices, its total fabrication time is reduced from over 3 h to ≈10 min. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Nonequilibrium phase transitions in cuprates observed by ultrafast electron crystallography.

PubMed

Gedik, Nuh; Yang, Ding-Shyue; Logvenov, Gennady; Bozovic, Ivan; Zewail, Ahmed H

2007-04-20

Nonequilibrium phase transitions, which are defined by the formation of macroscopic transient domains, are optically dark and cannot be observed through conventional temperature- or pressure-change studies. We have directly determined the structural dynamics of such a nonequilibrium phase transition in a cuprate superconductor. Ultrafast electron crystallography with the use of a tilted optical geometry technique afforded the necessary atomic-scale spatial and temporal resolutions. The observed transient behavior displays a notable "structural isosbestic" point and a threshold effect for the dependence of c-axis expansion (Deltac) on fluence (F), with Deltac/F = 0.02 angstrom/(millijoule per square centimeter). This threshold for photon doping occurs at approximately 0.12 photons per copper site, which is unexpectedly close to the density (per site) of chemically doped carriers needed to induce superconductivity.

Ultrafast gigantic photo-response in (EDO-TTF)2PF6 initiated by 10-fs laser pulses

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

Schoenlein, Robert William; Itatani, Jiro; Rini, Matteo

2006-08-07

We photo-exited a charge-ordered organic salt (EDO-TTF)2PF6 with sub-10-fs optical pulses. The photo-induced metallic phase appeared within 80-fs after pumping, characterized by large changes in reflectivity (DELTA R/R~0.8) followed by strong coherent phonon modulation

Negative effect of nanoconfinement on water transport across nanotube membranes

NASA Astrophysics Data System (ADS)

Zhao, Kuiwen; Wu, Huiying; Han, Baosan

2017-10-01

Nanoconfinement environments are commonly considered advantageous for ultrafast water flow across nanotube membranes. This study illustrates that nanoconfinement has a negative effect on water transport across nanotube membranes based on molecular dynamics simulations. Although water viscosity and the friction coefficient evidently decrease because of nanoconfinement, water molecular flux and flow velocity across carbon nanotubes decrease sharply with the pore size of nanotubes. The enhancement of water flow across nanotubes induced by the decreased friction coefficient and water viscosity is markedly less prominent than the negative effect induced by the increased flow barrier as the nanotube size decreases. The decrease in water flow velocity with the pore size of nanotubes indicates that nanoconfinement is not essential for the ultrafast flow phenomenon. In addition, the relationship between flow velocity and water viscosity at different temperatures is investigated at different temperatures. The results indicate that flow velocity is inversely proportional to viscosity for nanotubes with a pore diameter above 1 nm, thereby indicating that viscosity is still an effective parameter for describing the effect of temperature on the fluid transport at the nanoscale.

Ultrafast single molecule technique for the study of force dependent kinetics and conformational changes of actin-protein interaction involved in mechanotransduction

NASA Astrophysics Data System (ADS)

Sergides, M.; Arbore, C.; Pavone, F. S.; Capitanio, M.

2018-02-01

Mechanical signals occurring at the interface between cell membrane and extracellular matrix and at intercellular junctions trigger biochemical signals that are fundamental for cell growth, development and regulation. Adaptor proteins, which link the cell membrane to the actin cytoskeleton, seem to partake in this process of mechanotransduction. In particular, catenins play a key role in intercellular junctions, where they act as a bridge between the cell membrane and actin. Studies suggest that α-catenin contains a domain that normally masks vinculin binding sites, which can become accessible after a conformational change induced by an external force. Here we demonstrate a single-molecule technique for investigating actin-protein interactions at different forces (up to 17 pN) with adequate temporal resolution (sub-ms). This system is based on the ultrafast force-clamp spectroscopy technique that has been recently developed by our group and is adapted to study and measure force-dependent kinetics of the catenin-actin interaction, as well as the amplitude of the expected conformational changes such as force-induced protein unfolding.

Energetic mid-IR femtosecond pulse generation by self-defocusing soliton-induced dispersive waves in a bulk quadratic nonlinear crystal.

PubMed

Zhou, Binbin; Guo, Hairun; Bache, Morten

2015-03-09

Generating energetic femtosecond mid-IR pulses is crucial for ultrafast spectroscopy, and currently relies on parametric processes that, while efficient, are also complex. Here we experimentally show a simple alternative that uses a single pump wavelength without any pump synchronization and without critical phase-matching requirements. Pumping a bulk quadratic nonlinear crystal (unpoled LiNbO(3) cut for noncritical phase-mismatched interaction) with sub-mJ near-IR 50-fs pulses, tunable and broadband (∼ 1,000 cm(-1)) mid-IR pulses around 3.0 μm are generated with excellent spatio-temporal pulse quality, having up to 10.5 μJ energy (6.3% conversion). The mid-IR pulses are dispersive waves phase-matched to near-IR self-defocusing solitons created by the induced self-defocusing cascaded nonlinearity. This process is filament-free and the input pulse energy can therefore be scaled arbitrarily by using large-aperture crystals. The technique can readily be implemented with other crystals and laser wavelengths, and can therefore potentially replace current ultrafast frequency-conversion processes to the mid-IR.

Ultra-Fast Hadronic Calorimetry

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

Denisov, Dmitri; Lukić, Strahinja; Mokhov, Nikolai

2018-08-01

Calorimeters for particle physics experiments with integration time of a few ns will substantially improve the capability of the experiment to resolve event pileup and to reject backgrounds. In this paper the time development of hadronic showers induced by 30 and 60 GeV positive pions and 120 GeV protons is studied using Monte Carlo simulation and beam tests with a prototype of a sampling steel-scintillator hadronic calorimeter. In the beam tests, scintillator signals induced by hadronic showers in steel are sampled with a period of 0.2 ns and precisely time-aligned in order to study the average signal waveform at various locations with respectmore » to the beam particle impact. Simulations of the same setup are performed using the MARS15 code. Both simulation and test beam results suggest that energy deposition in steel calorimeters develop over a time shorter than 2 ns providing opportunity for ultra-fast calorimetry. Simulation results for an “ideal” calorimeter consisting exclusively of bulk tungsten or copper are presented to establish the lower limit of the signal integration window.« less

Ultra-Fast Hadronic Calorimetry

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

Denisov, Dmitri; Lukić, Strahinja; Mokhov, Nikolai

2017-12-18

Calorimeters for particle physics experiments with integration time of a few ns will substantially improve the capability of the experiment to resolve event pileup and to reject backgrounds. In this paper time development of hadronic showers induced by 30 and 60 GeV positive pions and 120 GeV protons is studied using Monte Carlo simulation and beam tests with a prototype of a sampling steel-scintillator hadronic calorimeter. In the beam tests, scintillator signals induced by hadronic showers in steel are sampled with a period of 0.2 ns and precisely time-aligned in order to study the average signal waveform at various locationsmore » w.r.t. the beam particle impact. Simulations of the same setup are performed using the MARS15 code. Both simulation and test beam results suggest that energy deposition in steel calorimeters develop over a time shorter than 3 ns providing opportunity for ultra-fast calorimetry. Simulation results for an "ideal" calorimeter consisting exclusively of bulk tungsten or copper are presented to establish the lower limit of the signal integration window.« less

Ultra-fast hadronic calorimetry

DOE PAGES

Denisov, Dmitri; Lukic, Strahinja; Mokhov, Nikolai; ...

2018-05-08

Calorimeters for particle physics experiments with integration time of a few ns will substantially improve the capability of the experiment to resolve event pileup and to reject backgrounds. In this paper the time development of hadronic showers induced by 30 and 60 GeV positive pions and 120 GeV protons is studied using Monte Carlo simulation and beam tests with a prototype of a sampling steel-scintillator hadronic calorimeter. In the beam tests, scintillator signals induced by hadronic showers in steel are sampled with a period of 0.2 ns and precisely time-aligned in order to study the average signal waveform at various locations with respectmore » to the beam particle impact. Simulations of the same setup are performed using the MARS15 code. Both simulation and test beam results suggest that energy deposition in steel calorimeters develop over a time shorter than 2 ns providing opportunity for ultra-fast calorimetry. As a result, simulation results for an “ideal” calorimeter consisting exclusively of bulk tungsten or copper are presented to establish the lower limit of the signal integration window.« less

Ultrafast Dynamics of a Nucleobase Analogue Illuminated by a Short Intense X-ray Free Electron Laser Pulse

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

Nagaya, K.; Motomura, K.; Kukk, E.

Understanding x-ray radiation damage is a crucial issue for both medical applications of x rays and x-ray free-electron-laser (XFEL) science aimed at molecular imaging. Decrypting the charge and fragmentation dynamics of nucleobases, the smallest units of a macro-biomolecule, contributes to a bottom-up understanding of the damage via cascades of phenomena following x-ray exposure. We investigate experimentally and by numerical simulations the ultrafast radiation damage induced on a nucleobase analogue (5-iodouracil) by an ultrashort (10 fs) high-intensity radiation pulse generated by XFEL at SPring-8 Angstrom Compact free electron Laser (SACLA). The present study elucidates a plausible underlying radiosensitizing mechanism of 5-iodouracil.more » This mechanism is independent of the exact composition of 5-iodouracil and thus relevant to other such radiosensitizers. Furthermore, we found that despite a rapid increase of the net molecular charge in the presence of iodine, and of the ultrafast release of hydrogen, the other atoms are almost frozen within the 10-fs duration of the exposure. Finally, this validates single-shot molecular imaging as a consistent approach, provided the radiation pulse used is brief enough.« less

Ultrafast Dynamics of a Nucleobase Analogue Illuminated by a Short Intense X-ray Free Electron Laser Pulse

DOE PAGES

Nagaya, K.; Motomura, K.; Kukk, E.; ...

2016-06-16

Understanding x-ray radiation damage is a crucial issue for both medical applications of x rays and x-ray free-electron-laser (XFEL) science aimed at molecular imaging. Decrypting the charge and fragmentation dynamics of nucleobases, the smallest units of a macro-biomolecule, contributes to a bottom-up understanding of the damage via cascades of phenomena following x-ray exposure. We investigate experimentally and by numerical simulations the ultrafast radiation damage induced on a nucleobase analogue (5-iodouracil) by an ultrashort (10 fs) high-intensity radiation pulse generated by XFEL at SPring-8 Angstrom Compact free electron Laser (SACLA). The present study elucidates a plausible underlying radiosensitizing mechanism of 5-iodouracil.more » This mechanism is independent of the exact composition of 5-iodouracil and thus relevant to other such radiosensitizers. Furthermore, we found that despite a rapid increase of the net molecular charge in the presence of iodine, and of the ultrafast release of hydrogen, the other atoms are almost frozen within the 10-fs duration of the exposure. Finally, this validates single-shot molecular imaging as a consistent approach, provided the radiation pulse used is brief enough.« less

Electron theory of fast and ultrafast dissipative magnetization dynamics.

PubMed

Fähnle, M; Illg, C

2011-12-14

For metallic magnets we review the experimental and electron-theoretical investigations of fast magnetization dynamics (on a timescale of ns to 100 ps) and of laser-pulse-induced ultrafast dynamics (few hundred fs). It is argued that for both situations the dominant contributions to the dissipative part of the dynamics arise from the excitation of electron-hole pairs and from the subsequent relaxation of these pairs by spin-dependent scattering processes, which transfer angular momentum to the lattice. By effective field theories (generalized breathing and bubbling Fermi-surface models) it is shown that the Gilbert equation of motion, which is often used to describe the fast dissipative magnetization dynamics, must be extended in several aspects. The basic assumptions of the Elliott-Yafet theory, which is often used to describe the ultrafast spin relaxation after laser-pulse irradiation, are discussed very critically. However, it is shown that for Ni this theory probably yields a value for the spin-relaxation time T(1) in good agreement with the experimental value. A relation between the quantity α characterizing the damping of the fast dynamics in simple situations and the time T(1) is derived. © 2011 IOP Publishing Ltd

Effects of iron on the lattice thermal conductivity of Earth's deep mantle and implications for mantle dynamics

NASA Astrophysics Data System (ADS)

Hsieh, Wen-Pin; Deschamps, Frédéric; Okuchi, Takuo; Lin, Jung-Fu

2018-04-01

Iron may critically influence the physical properties and thermochemical structures of Earth's lower mantle. Its effects on thermal conductivity, with possible consequences on heat transfer and mantle dynamics, however, remain largely unknown. We measured the lattice thermal conductivity of lower-mantle ferropericlase to 120 GPa using the ultrafast optical pump-probe technique in a diamond anvil cell. The thermal conductivity of ferropericlase with 56% iron significantly drops by a factor of 1.8 across the spin transition around 53 GPa, while that with 8–10% iron increases monotonically with pressure, causing an enhanced iron substitution effect in the low-spin state. Combined with bridgmanite data, modeling of our results provides a self-consistent radial profile of lower-mantle thermal conductivity, which is dominated by pressure, temperature, and iron effects, and shows a twofold increase from top to bottom of the lower mantle. Such increase in thermal conductivity may delay the cooling of the core, while its decrease with iron content may enhance the dynamics of large low shear-wave velocity provinces. Our findings further show that, if hot and strongly enriched in iron, the seismic ultralow velocity zones have exceptionally low conductivity, thus delaying their cooling.

Effects of iron on the lattice thermal conductivity of Earth's deep mantle and implications for mantle dynamics.

PubMed

Hsieh, Wen-Pin; Deschamps, Frédéric; Okuchi, Takuo; Lin, Jung-Fu

2018-04-17

Iron may critically influence the physical properties and thermochemical structures of Earth's lower mantle. Its effects on thermal conductivity, with possible consequences on heat transfer and mantle dynamics, however, remain largely unknown. We measured the lattice thermal conductivity of lower-mantle ferropericlase to 120 GPa using the ultrafast optical pump-probe technique in a diamond anvil cell. The thermal conductivity of ferropericlase with 56% iron significantly drops by a factor of 1.8 across the spin transition around 53 GPa, while that with 8-10% iron increases monotonically with pressure, causing an enhanced iron substitution effect in the low-spin state. Combined with bridgmanite data, modeling of our results provides a self-consistent radial profile of lower-mantle thermal conductivity, which is dominated by pressure, temperature, and iron effects, and shows a twofold increase from top to bottom of the lower mantle. Such increase in thermal conductivity may delay the cooling of the core, while its decrease with iron content may enhance the dynamics of large low shear-wave velocity provinces. Our findings further show that, if hot and strongly enriched in iron, the seismic ultralow velocity zones have exceptionally low conductivity, thus delaying their cooling.

The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales (A "Life at the Frontiers of Energy Research" contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum)

ScienceCinema

Mao, Ho-kwang (Director, Center for Energy Frontier Research in Extreme Environments); EFree Staff

2017-12-09

'The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales ' was submitted by the Center for Energy Frontier Research in Extreme Environments (EFree) to the 'Life at the Frontiers of Energy Research' video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. EFree is directed by Ho-kwang Mao at the Carnegie Institute of Washington and is a partnership of scientists from thirteen institutions.The Office of Basic Energy Sciences in the U.S. Department of Energy's Office of Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges. The mission of Energy Frontier Research in Extreme Environments is 'to accelerate the discovery and creation of energy-relevant materials using extreme pressures and temperatures.' Research topics are: catalysis (CO{sub 2}, water), photocatalysis, solid state lighting, optics, thermelectric, phonons, thermal conductivity, solar electrodes, fuel cells, superconductivity, extreme environment, radiation effects, defects, spin dynamics, CO{sub 2} (capture, convert, store), greenhouse gas, hydrogen (fuel, storage), ultrafast physics, novel materials synthesis, and defect tolerant materials.

Ultrafast Nanoscale Raman Thermometry Proves Heating Is Not a Primary Mechanism for Plasmon-Driven Photocatalysis.

PubMed

Keller, Emily L; Frontiera, Renee R

2018-06-08

Plasmonic materials efficiently convert light to various forms of energies for many applications, including photocatalysis, photovoltaics, and photothermal therapies. In particular, plasmonic photocatalysts hold incredible promise for highly selective sunlight-driven catalysis through the generation of highly energetic holes and electrons used to drive chemical reactions. However, plasmons are also known to generate heat, and the partitioning of photoexcitation energy into hot carriers and heat on molecularly relevant time scales is not well understood, yet plays a crucial role in designing and understanding these photocatalysts. Using an ultrafast surface-enhanced Raman thermometry technique, we probe the effective temperature, equivalent to the mode-specific increase of vibrational kinetic energy, of molecules adsorbed to gold nanoparticle aggregates in the most active hot spots on the picosecond time scale of chemical reactivity. This represents the first measurement of vibrational energy deposition for coupled molecular-plasmonic systems on the picosecond time scale of molecular motion. We find that upon plasmon excitation, the adsorbates in the hot spots undergo an initial energy transfer within several picoseconds that changes the effective temperature of the system by less than 100 K, even at peak flux values 10 8 times stronger than focused sunlight. The energy quickly dissipates from the adsorbates into the surroundings in less than 5 ps, even at the highest values of photoexcitation. This surprisingly modest energy transfer of the most active regions of the plasmonic materials on the ultrafast time scale decisively proves that most plasmonic photocatalysis is not primarily thermally driven.

The Investigation of New Magnetic Materials and Their Phenomena Using Ultrafast Fresnel Transmission Electron Microscopy

NASA Astrophysics Data System (ADS)

Schliep, Karl B.

State-of-the-art technology drives scientific progress, pushing the boundaries of our current understanding of fundamental processes and mechanisms. Our continual scientific advancement is hindered only by what we can observe and experimentally verify; thus, it is reasonable to assert that instrument development and improvement is the cornerstone for technological and intellectual growth. For example, the invention of transmission electron microscopy (TEM) allowed us to observe nanoscale phenomena for the first time in the 1930s and even now it is invaluable in the development of smaller, faster electronics. As we uncover more about the fundamentals of nanoscale phenomena, we have realized that images alone reveal only a snapshot of the story; to continue progressing we need a way to observe the entire scene unfold (e.g. how defects affect the flow of current across a transistor or how thermal energy propagates in nanoscale systems like graphene). Recently, by combining the spatial resolution of a TEM with the temporal resolution of ultrafast lasers, ultrafast electron microscopy ? or microscope ? (UEM) has allowed us to simultaneously observe transient nanoscale phenomena at ultrafast timescales. Ultrafast characterization techniques allow for the investigation of a new realm of previously unseen phenomenon inherent to the transient electronic, magnetic, and structural properties of materials. However, despite the progress made in ultrafast techniques, capturing the nanoscale spatial sub-ns temporal mechanisms and phenomenon at play in magnetic materials (especially during the operation of magnetic devices) has only recently become possible using UEM. With only a handful of instruments available, magnetic characterization using UEM is far from commonplace and any advances made are sparsely reported, and further, specific to the individual instrument. In this dissertation, I outline the development of novel magnetic materials and the establishment of a UEM lab at the University of Minnesota and how I explored the application of it toward the investigation of magnetic materials. In my discussion of UEM, I have made a concerted effort to highlight the unique challenges faced when getting a UEM lab running so that new researchers may circumvent these challenges. Of note in my graduate studies, I assisted in the development of three different magnetic material systems, strained Fe nanoparticles for permanent magnetic applications, FePd for applications in spintronic devices, and a rare-earth transition-metal (RE-TM) alloy that exhibits new magneto-optic phenomena. In studying the morphological and magnetic effects of lasers on these RE-TM alloys using the in situ laser irradiation capabilities of UEM along with standard TEM techniques and computational modeling, I uncovered a possible limitation in their utility for memory applications. Furthermore, with the aid of particle tracing software, I was able to optimize our UEM system for magnetic imaging and demonstrate the resolution of ultrafast demagnetization using UEM.

Ab initio nonadiabatic molecular dynamics of the ultrafast electron injection from a PbSe quantum dot into the TiO2 surface.

PubMed

Long, Run; Prezhdo, Oleg V

2011-11-30

Following recent experiments [Science 2010, 328, 1543; PNAS 2011, 108, 965], we report an ab initio nonadiabatic molecular dynamics (NAMD) simulation of the ultrafast photoinduced electron transfer (ET) from a PbSe quantum dot (QD) into the rutile TiO(2) (110) surface. The system forms the basis for QD-sensitized semiconductor solar cells and demonstrates that ultrafast interfacial ET is instrumental for achieving high efficiencies in solar-to-electrical energy conversion. The simulation supports the observation that the ET successfully competes with energy losses due to electron-phonon relaxation. The ET proceeds by the adiabatic mechanism because of strong donor-acceptor coupling. High frequency polar vibrations of both QD and TiO(2) promote the ET, since these modes can rapidly influence the donor-acceptor state energies and coupling. Low frequency vibrations generate a distribution of initial conditions for ET, which shows a broad variety of scenarios at the single-molecule level. Compared to the molecule-TiO(2) interfaces, the QD-TiO(2) system exhibits pronounced differences that arise due to the larger size and higher rigidity of QDs relative to molecules. Both donor and acceptor states are more delocalized in the QD system, and the ET is promoted by optical phonons, which have relatively low frequencies in the QD materials composed of heavy elements. In contrast, in molecular systems, optical phonons are not thermally accessible under ambient conditions. Meanwhile, TiO(2) acceptor states resemble surface impurities due to the local influence of molecular chromophores. At the same time, the photoinduced ET at both QD-TiO(2) and molecule-TiO(2) interfaces is ultrafast and occurs by the adiabatic mechanism, as a result of strong donor-acceptor coupling. The reported state-of-the-art simulation generates a detailed time-domain atomistic description of the interfacial ET process that is fundamental to a wide variety of applications.

Electrochemically exfoliated graphene as a novel microwave susceptor: the ultrafast microwave-assisted synthesis of carbon-coated silicon-graphene film as a lithium-ion battery anode.

PubMed

Kim, Jong Min; Ko, Dongjin; Oh, Jiseop; Lee, Jeongyeon; Hwang, Taejin; Jeon, Youngmoo; Hooch Antink, Wytse; Piao, Yuanzhe

2017-10-19

Graphene nanocomposites have attracted much attention in many applications due to their superior properties. However, preparing graphene nanocomposites requires a time-consuming thermal treatment to reduce the graphene or synthesize nanomaterials, in most cases. We present an ultrafast synthesis of a carbon-coated silicon-graphene nanocomposite using a commercial microwave system. Electrochemically exfoliated graphene is used as a novel microwave susceptor to deliver efficient microwave energy conversion. Unlike graphene oxide, it does not require a time-consuming pre-thermal reduction or toxic chemical reduction to absorb microwave radiation efficiently. A carbon-coated silicon nanoparticle-electrochemically exfoliated graphene nanocomposite film was prepared by a few seconds' microwave irradiation. The sp 2 domains of graphene absorb microwave radiation and generate heat to simultaneously reduce the graphene and carbonize the polydopamine carbon precursor. The as-prepared N-doped carbon-coated silicon-graphene film was used as a lithium-ion battery anode. The N-doped carbon coating decreases the contact resistance between silicon nanoparticles and graphene provides a wide range conductive network. Consequently, it exhibited a reversible capacity of 1744 mA h g -1 at a current density of 0.1 A g -1 and 662 mA h g -1 at 1.0 A g -1 after 200 cycles. This method can potentially be a general approach to prepare various graphene nanocomposites in an extremely short time.

Compression selective solid-state chemistry

NASA Astrophysics Data System (ADS)

Hu, Anguang

Compression selective solid-state chemistry refers to mechanically induced selective reactions of solids under thermomechanical extreme conditions. Advanced quantum solid-state chemistry simulations, based on density functional theory with localized basis functions, were performed to provide a remarkable insight into bonding pathways of high-pressure chemical reactions in all agreement with experiments. These pathways clearly demonstrate reaction mechanisms in unprecedented structural details, showing not only the chemical identity of reactive intermediates but also how atoms move along the reaction coordinate associated with a specific vibrational mode, directed by induced chemical stress occurred during bond breaking and forming. It indicates that chemical bonds in solids can break and form precisely under compression as we wish. This can be realized through strongly coupling of mechanical work to an initiation vibrational mode when all other modes can be suppressed under compression, resulting in ultrafast reactions to take place isothermally in a few femtoseconds. Thermodynamically, such reactions correspond to an entropy minimum process on an isotherm where the compression can force thermal expansion coefficient equal to zero. Combining a significantly brief reaction process with specific mode selectivity, both statistical laws and quantum uncertainty principle can be bypassed to precisely break chemical bonds, establishing fundamental principles of compression selective solid-state chemistry. Naturally this leads to understand the ''alchemy'' to purify, grow, and perfect certain materials such as emerging novel disruptive energetics.

Heterogeneous nucleation and growth dynamics in the light-induced phase transition in vanadium dioxide

DOE PAGES

Brady, Nathaniel F.; Appavoo, Kannatassen; Seo, Minah; ...

2016-03-02

Here we report on ultrafast optical investigations of the light-induced insulator-to-metal phase transition in vanadium dioxide with controlled disorder generated by substrate mismatch. These results reveal common dynamics of this optically-induced phase transition that are independent of this disorder. Lastly, above the fluence threshold for completing the transition to the rutile crystalline phase, we find a common time scale, independent of sample morphology, of 40.5 ± 2 ps that is consistent with nucleation and growth dynamics of the R phase from the parent M1 ground state.

Laser-Induced Skyrmion Writing and Erasing in an Ultrafast Cryo-Lorentz Transmission Electron Microscope

NASA Astrophysics Data System (ADS)

Berruto, G.; Madan, I.; Murooka, Y.; Vanacore, G. M.; Pomarico, E.; Rajeswari, J.; Lamb, R.; Huang, P.; Kruchkov, A. J.; Togawa, Y.; LaGrange, T.; McGrouther, D.; Rønnow, H. M.; Carbone, F.

2018-03-01

We demonstrate that light-induced heat pulses of different duration and energy can write Skyrmions in a broad range of temperatures and magnetic field in FeGe. Using a combination of camera-rate and pump-probe cryo-Lorentz transmission electron microscopy, we directly resolve the spatiotemporal evolution of the magnetization ensuing optical excitation. The Skyrmion lattice was found to maintain its structural properties during the laser-induced demagnetization, and its recovery to the initial state happened in the sub-μ s to μ s range, depending on the cooling rate of the system.

The ultrafast dynamics and conductivity of photoexcited graphene at different Fermi energies

PubMed Central

Turchinovich, Dmitry; Kläui, Mathias; Hendry, Euan; Polini, Marco

2018-01-01

For many of the envisioned optoelectronic applications of graphene, it is crucial to understand the subpicosecond carrier dynamics immediately following photoexcitation and the effect of photoexcitation on the electrical conductivity—the photoconductivity. Whereas these topics have been studied using various ultrafast experiments and theoretical approaches, controversial and incomplete explanations concerning the sign of the photoconductivity, the occurrence and significance of the creation of additional electron-hole pairs, and, in particular, how the relevant processes depend on Fermi energy have been put forward. We present a unified and intuitive physical picture of the ultrafast carrier dynamics and the photoconductivity, combining optical pump–terahertz probe measurements on a gate-tunable graphene device, with numerical calculations using the Boltzmann equation. We distinguish two types of ultrafast photo-induced carrier heating processes: At low (equilibrium) Fermi energy (EF ≲ 0.1 eV for our experiments), broadening of the carrier distribution involves interband transitions (interband heating). At higher Fermi energy (EF ≳ 0.15 eV), broadening of the carrier distribution involves intraband transitions (intraband heating). Under certain conditions, additional electron-hole pairs can be created [carrier multiplication (CM)] for low EF, and hot carriers (hot-CM) for higher EF. The resultant photoconductivity is positive (negative) for low (high) EF, which in our physical picture, is explained using solely electronic effects: It follows from the effect of the heated carrier distributions on the screening of impurities, consistent with the DC conductivity being mostly due to impurity scattering. The importance of these insights is highlighted by a discussion of the implications for graphene photodetector applications. PMID:29756035

Ultrafast-laser dicing of thin silicon wafers: strategies to improve front- and backside breaking strength

NASA Astrophysics Data System (ADS)

Domke, Matthias; Egle, Bernadette; Stroj, Sandra; Bodea, Marius; Schwarz, Elisabeth; Fasching, Gernot

2017-12-01

Thin 50-µm silicon wafers are used to improve heat dissipation of chips with high power densities. However, mechanical dicing methods cause chipping at the edges of the separated dies that reduce the mechanical stability. Thermal load changes may then lead to sudden chip failure. Recent investigations showed that the mechanical stability of the cut chips could be increased using ultrashort-pulsed lasers, but only at the laser entrance (front) side and not at the exit (back) side. The goal of this study was to find strategies to improve both front- and backside breaking strength of chips that were cut out of an 8″ wafer with power metallization using an ultrafast laser. In a first experiment, chips were cut by scanning the laser beam in single lines across the wafer using varying fluencies and scan speeds. Three-point bending tests of the cut chips were performed to measure front and backside breaking strengths. The results showed that the breaking strength of both sides increased with decreasing accumulated fluence per scan. Maximum breaking strengths of about 1100 MPa were achieved at the front side, but only below 600 MPa were measured for the backside. A second experiment was carried out to optimize the backside breaking strength. Here, parallel line scans to increase the distance between separated dies and step cuts to minimize the effect of decreasing fluence during scribing were performed. Bending tests revealed that breaking strengths of about 1100 MPa could be achieved also on the backside using the step cut. A reason for the superior performance could be found by calculating the fluence absorbed by the sidewalls. The calculations suggested that an optimal fluence level to minimize thermal side effects and periodic surface structures was achieved due to the step cut. Remarkably, the best breaking strengths values achieved in this study were even higher than the values obtained on state of the art ns-laser and mechanical dicing machines. This is the first study to the knowledge of the authors, which demonstrates that ultrafast-laser dicing improves the mechanical stability of thin silicon chips.

Kinetic Analysis of Benign and Malignant Breast Lesions With Ultrafast Dynamic Contrast-Enhanced MRI: Comparison With Standard Kinetic Assessment.

PubMed

Abe, Hiroyuki; Mori, Naoko; Tsuchiya, Keiko; Schacht, David V; Pineda, Federico D; Jiang, Yulei; Karczmar, Gregory S

2016-11-01

The purposes of this study were to evaluate diagnostic parameters measured with ultrafast MRI acquisition and with standard acquisition and to compare diagnostic utility for differentiating benign from malignant lesions. Ultrafast acquisition is a high-temporal-resolution (7 seconds) imaging technique for obtaining 3D whole-breast images. The dynamic contrast-enhanced 3-T MRI protocol consists of an unenhanced standard and an ultrafast acquisition that includes eight contrast-enhanced ultrafast images and four standard images. Retrospective assessment was performed for 60 patients with 33 malignant and 29 benign lesions. A computer-aided detection system was used to obtain initial enhancement rate and signal enhancement ratio (SER) by means of identification of a voxel showing the highest signal intensity in the first phase of standard imaging. From the same voxel, the enhancement rate at each time point of the ultrafast acquisition and the AUC of the kinetic curve from zero to each time point of ultrafast imaging were obtained. There was a statistically significant difference between benign and malignant lesions in enhancement rate and kinetic AUC for ultrafast imaging and also in initial enhancement rate and SER for standard imaging. ROC analysis showed no significant differences between enhancement rate in ultrafast imaging and SER or initial enhancement rate in standard imaging. Ultrafast imaging is useful for discriminating benign from malignant lesions. The differential utility of ultrafast imaging is comparable to that of standard kinetic assessment in a shorter study time.

Laser-Induced Ultrafast Demagnetization: Femtomagnetism, a New Frontier?

NASA Astrophysics Data System (ADS)

Zhang, Guoping; Huebner, Wolfgang; Beaurepaire, Eric; Bigot, Jean-Yves

The conventional demagnetization process (spin precession, magnetic domain motion and rotation) is governed mainly by spin-lattice, magnetic dipole and Zeeman, and spin-spin interactions. It occurs on a timescale of nanoseconds. Technologically, much faster magnetization changes are always in great demand to improve data processing speed. Unfortunately, the present speed of magnetic devices is already at the limit of the conventional mechanism with little room left. Fortunately and unprecedentedly, recent experimental investigations have evidenced much faster magnetization dynamics which occurs on a femtosecond time scale: femtomagnetism. This novel spin dynamics has not been well-understood until now. This article reviews the current status of ultrafast spin dynamics and presents a perspective for future experimental and theoretical investigations.Present address: Department of Physics and Astronomy, The University of Tennessee at Knoxville, TN 37996-1200, USA; gpzhang@utk.edu

Ultrafast myoglobin structural dynamics observed with an X-ray free-electron laser

DOE PAGES

Levantino, Matteo; Schirò, Giorgio; Lemke, Henrik Till; ...

2015-04-02

Light absorption can trigger biologically relevant protein conformational changes. The light induced structural rearrangement at the level of a photoexcited chromophore is known to occur in the femtosecond timescale and is expected to propagate through the protein as a quake-like intramolecular motion. Here we report direct experimental evidence of such ‘proteinquake’ observed in myoglobin through femtosecond X-ray solution scattering measurements performed at the Linac Coherent Light Source X-ray free-electron laser. An ultrafast increase of myoglobin radius of gyration occurs within 1 picosecond and is followed by a delayed protein expansion. As the system approaches equilibrium it undergoes damped oscillations withmore » a ~3.6-picosecond time period. Our results unambiguously show how initially localized chemical changes can propagate at the level of the global protein conformation in the picosecond timescale.« less

Ultrafast proton radiography of the magnetic fields generated by a laser-driven coil current

DOE PAGES

Gao, Lan; Ji, Hantao; Fiksel, Gennady; ...

2016-04-15

Magnetic fields generated by a current flowing through a U-shaped coil connecting two copper foils were measured using ultrafast proton radiography. Two ~ 1.25 kJ, 1-ns laser pulses propagated through laser entrance holes in the front foil and were focused to the back foil with an intensity of ~ 3 x 10 16 W/cm 2. The intense laser-solid interaction induced a high voltage between the copper foils and generated a large current in the connecting coil. The proton data show ~ 40-50 T magnetic fields at the center of the coil ~ 3-4 ns after laser irradiation. In conclusion, themore » experiments provide significant insight for future target designs that aim to develop a powerful source of external magnetic fields for various applications in high-energy-density science.« less

Collapse of superconductivity in cuprates via ultrafast quenching of phase coherence

DOE PAGES

Boschini, F.; da Silva Neto, E. H.; Razzoli, E.; ...

2018-04-02

The possibility of driving phase transitions in low-density condensates through the loss of phase coherence alone has far-reaching implications for the study of quantum phases of matter. This has inspired the development of tools to control and explore the collective properties of condensate phases via phase fluctuations. Electrically gated oxide interfaces, ultracold Fermi atoms and cuprate superconductors, which are characterized by an intrinsically small phase stiffness, are paradigmatic examples where these tools are having a dramatic impact. In this study, we use light pulses shorter than the internal thermalization time to drive and probe the phase fragility of the Bimore » 2Sr 2CaCu 2O 8+δ cuprate superconductor, completely melting the superconducting condensate without affecting the pairing strength. The resulting ultrafast dynamics of phase fluctuations and charge excitations are captured and disentangled by time-resolved photoemission spectroscopy. This work demonstrates the dominant role of phase coherence in the superconductor-to-normal state phase transition and offers a benchmark for non-equilibrium spectroscopic investigations of the cuprate phase diagram.« less

Microscopic origins of the terahertz carrier relaxation and cooling dynamics in graphene

PubMed Central

Mihnev, Momchil T.; Kadi, Faris; Divin, Charles J.; Winzer, Torben; Lee, Seunghyun; Liu, Che-Hung; Zhong, Zhaohui; Berger, Claire; de Heer, Walt A.; Malic, Ermin; Knorr, Andreas; Norris, Theodore B.

2016-01-01

The ultrafast dynamics of hot carriers in graphene are key to both understanding of fundamental carrier–carrier interactions and carrier–phonon relaxation processes in two-dimensional materials, and understanding of the physics underlying novel high-speed electronic and optoelectronic devices. Many recent experiments on hot carriers using terahertz spectroscopy and related techniques have interpreted the variety of observed signals within phenomenological frameworks, and sometimes invoke extrinsic effects such as disorder. Here, we present an integrated experimental and theoretical programme, using ultrafast time-resolved terahertz spectroscopy combined with microscopic modelling, to systematically investigate the hot-carrier dynamics in a wide array of graphene samples having varying amounts of disorder and with either high or low doping levels. The theory reproduces the observed dynamics quantitatively without the need to invoke any fitting parameters, phenomenological models or extrinsic effects such as disorder. We demonstrate that the dynamics are dominated by the combined effect of efficient carrier–carrier scattering, which maintains a thermalized carrier distribution, and carrier–optical–phonon scattering, which removes energy from the carrier liquid. PMID:27221060

Collapse of superconductivity in cuprates via ultrafast quenching of phase coherence

NASA Astrophysics Data System (ADS)

Boschini, F.; da Silva Neto, E. H.; Razzoli, E.; Zonno, M.; Peli, S.; Day, R. P.; Michiardi, M.; Schneider, M.; Zwartsenberg, B.; Nigge, P.; Zhong, R. D.; Schneeloch, J.; Gu, G. D.; Zhdanovich, S.; Mills, A. K.; Levy, G.; Jones, D. J.; Giannetti, C.; Damascelli, A.

2018-05-01

The possibility of driving phase transitions in low-density condensates through the loss of phase coherence alone has far-reaching implications for the study of quantum phases of matter. This has inspired the development of tools to control and explore the collective properties of condensate phases via phase fluctuations. Electrically gated oxide interfaces1,2, ultracold Fermi atoms3,4 and cuprate superconductors5,6, which are characterized by an intrinsically small phase stiffness, are paradigmatic examples where these tools are having a dramatic impact. Here we use light pulses shorter than the internal thermalization time to drive and probe the phase fragility of the Bi2Sr2CaCu2O8+δ cuprate superconductor, completely melting the superconducting condensate without affecting the pairing strength. The resulting ultrafast dynamics of phase fluctuations and charge excitations are captured and disentangled by time-resolved photoemission spectroscopy. This work demonstrates the dominant role of phase coherence in the superconductor-to-normal state phase transition and offers a benchmark for non-equilibrium spectroscopic investigations of the cuprate phase diagram.

Collapse of superconductivity in cuprates via ultrafast quenching of phase coherence

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

Boschini, F.; da Silva Neto, E. H.; Razzoli, E.

The possibility of driving phase transitions in low-density condensates through the loss of phase coherence alone has far-reaching implications for the study of quantum phases of matter. This has inspired the development of tools to control and explore the collective properties of condensate phases via phase fluctuations. Electrically gated oxide interfaces, ultracold Fermi atoms and cuprate superconductors, which are characterized by an intrinsically small phase stiffness, are paradigmatic examples where these tools are having a dramatic impact. In this study, we use light pulses shorter than the internal thermalization time to drive and probe the phase fragility of the Bimore » 2Sr 2CaCu 2O 8+δ cuprate superconductor, completely melting the superconducting condensate without affecting the pairing strength. The resulting ultrafast dynamics of phase fluctuations and charge excitations are captured and disentangled by time-resolved photoemission spectroscopy. This work demonstrates the dominant role of phase coherence in the superconductor-to-normal state phase transition and offers a benchmark for non-equilibrium spectroscopic investigations of the cuprate phase diagram.« less

Scattering properties of ultrafast laser-induced refractive index shaping lenticular structures in hydrogels

NASA Astrophysics Data System (ADS)

Wozniak, Kaitlin T.; Germer, Thomas A.; Butler, Sam C.; Brooks, Daniel R.; Huxlin, Krystel R.; Ellis, Jonathan D.

2018-02-01

We present measurements of light scatter induced by a new ultrafast laser technique being developed for laser refractive correction in transparent ophthalmic materials such as cornea, contact lenses, and/or intraocular lenses. In this new technique, called intra-tissue refractive index shaping (IRIS), a 405 nm femtosecond laser is focused and scanned below the corneal surface, inducing a spatially-varying refractive index change that corrects vision errors. In contrast with traditional laser correction techniques, such as laser in-situ keratomileusis (LASIK) or photorefractive keratectomy (PRK), IRIS does not operate via photoablation, but rather changes the refractive index of transparent materials such as cornea and hydrogels. A concern with any laser eye correction technique is additional scatter induced by the process, which can adversely affect vision, especially at night. The goal of this investigation is to identify sources of scatter induced by IRIS and to mitigate possible effects on visual performance in ophthalmic applications. Preliminary light scattering measurements on patterns written into hydrogel showed four sources of scatter, differentiated by distinct behaviors: (1) scattering from scanned lines; (2) scattering from stitching errors, resulting from adjacent scanning fields not being aligned to one another; (3) diffraction from Fresnel zone discontinuities; and (4) long-period variations in the scans that created distinct diffraction peaks, likely due to inconsistent line spacing in the writing instrument. By knowing the nature of these different scattering errors, it will now be possible to modify and optimize the design of IRIS structures to mitigate potential deficits in visual performance in human clinical trials.

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 interest. With the emergence of new instruments such as X-ray free electron lasers (XFELs), it is now possible to perform ultrafast laser pump/X-ray emission probe experiments. In this case, one probes the density of occupied states. These core-level spectroscopies and other emerging ones, such as photoelectron spectroscopy of solutions, are delivering a hitherto unseen degree of detail into the photophysics of metal-based molecular complexes. In this Account, we will give examples of applications of the various methods listed above to address specific photophysical processes.

Modeling ultrafast laser-induced nanocavitation around plasmonic nanoparticles (Conference Presentation)

NASA Astrophysics Data System (ADS)

Meunier, Michel; Dagallier, Adrien; Lachaine, Rémi; Boutopoulos, Christos; Boulais, Étienne

2017-03-01

Vapor nanobubbles generated around plasmonic nanoparticles (NPs) by ultrafast laser irradiation are efficient for inducing localized damage to living cells. Killing targeted cancer cells or gene delivery can therefore be envisioned using this new technology [1,2]. The extent of the damage and its non-lethal character are linked to the size of the nanobubble. Precise understanding of the mechanisms leading to bubble formation around plasmonic nanostructures is necessary to optimize the technique. In this presentation, we present a complete model that successfully describes all interactions occurring during the irradiation of plasmonics nanostructures by an ultrafast laser of various pulse widths and fluences. Nanoavitation is caused by the interplay between heat conduction at the NP-medium interface and non-linear plasmon-enhanced photoionization of a nanoplasma in the near-field [3-5], the former being dominant for in-resonance and the latter for off-resonance irradiation. Modeling of the whole laser-nanoparticle interaction, together with the help of the shadowgraphic imaging and scattering techniques [3-5], give valuable insight on the mechanisms of cavitation at the nanoscale, leading to possible optimization of the nanostructure for bubble-based nanomedicine applications. 1- E. Boulais, R. Lachaine, A. Hatef, and M. Meunier, Journal of Photochemistry and Photobiology C: Photochemistry Reviews 17, 26-49 (2013). 2- E. Bergeron, S. Patskovsky, D. Rioux, and M. Meunier, Nanoscale 7,17836-17847 (2015). 3- E. Boulais, R. Lachaine, and M. Meunier, Nano Letters 12, 4763-4769 (2012). 4- R. Lachaine, E. Boulais, and M. Meunier, ACS Photonics 1, 331-336 (2014). 5- C. Boutopoulos, A. Hatef, M. Fortin-Deschênes, and M. Meunier Nanoscale 7,11758-11765 (2015).

Cationic 1,2,3-Triazolium Alkynes: Components To Enhance 1,4-Regioselective Azide-Alkyne Cycloaddition Reactions.

PubMed

Monasterio, Zaira; Sagartzazu-Aizpurua, Maialen; Miranda, José I; Reyes, Yuri; Aizpurua, Jesus M

2016-02-19

4-Alkynyl-1,2,3-triazolium cations undergo thermal [3 + 2] cycloaddition reactions with azides roughly 50- to 100-fold faster than comparable noncharged alkynes. Further, the reaction is highly 1,4-regioselective (dr up to 99:1) owing to the selective stabilization of 1,4-TS transition states via conjugative π-acceptor assistance of the alkyne triazolium ring. The novel cationic triazolium alkynes also accelerate the CuAAC reaction to provide bis(1,2,3-triazoles) in an "ultrafast" way (<5 min).

Nanoscale interfacial heat transport of ultrathin epitaxial hetero films: Few monolayer Pb(111) on Si(111)

NASA Astrophysics Data System (ADS)

Witte, T.; Frigge, T.; Hafke, B.; Krenzer, B.; Horn-von Hoegen, M.

2017-06-01

We studied the phononic heat transport from ultrathin epitaxial Pb(111) films across the heterointerface into a Si(111) substrate by means of ultrafast electron diffraction. The thickness of the Pb films was varied from 15 to 4 monolayers. It was found that the thermal boundary conductance σTBC of the heterointerface is independent of the film thickness. We have no evidence for finite size effects: the continuum description of heat transport is still valid, even for the thinnest films of only 4 monolayer thickness.

Thermal noise model of antiferromagnetic dynamics: A macroscopic approach

NASA Astrophysics Data System (ADS)

Li, Xilai; Semenov, Yuriy; Kim, Ki Wook

In the search for post-silicon technologies, antiferromagnetic (AFM) spintronics is receiving widespread attention. Due to faster dynamics when compared with its ferromagnetic counterpart, AFM enables ultra-fast magnetization switching and THz oscillations. A crucial factor that affects the stability of antiferromagnetic dynamics is the thermal fluctuation, rarely considered in AFM research. Here, we derive from theory both stochastic dynamic equations for the macroscopic AFM Neel vector (L-vector) and the corresponding Fokker-Plank equation for the L-vector distribution function. For the dynamic equation approach, thermal noise is modeled by a stochastic fluctuating magnetic field that affects the AFM dynamics. The field is correlated within the correlation time and the amplitude is derived from the energy dissipation theory. For the distribution function approach, the inertial behavior of AFM dynamics forces consideration of the generalized space, including both coordinates and velocities. Finally, applying the proposed thermal noise model, we analyze a particular case of L-vector reversal of AFM nanoparticles by voltage controlled perpendicular magnetic anisotropy (PMA) with a tailored pulse width. This work was supported, in part, by SRC/NRI SWAN.

Ultrafast and nonlinear surface-enhanced Raman spectroscopy.

PubMed

Gruenke, Natalie L; Cardinal, M Fernanda; McAnally, Michael O; Frontiera, Renee R; Schatz, George C; Van Duyne, Richard P

2016-04-21

Ultrafast surface-enhanced Raman spectroscopy (SERS) has the potential to study molecular dynamics near plasmonic surfaces to better understand plasmon-mediated chemical reactions such as plasmonically-enhanced photocatalytic or photovoltaic processes. This review discusses the combination of ultrafast Raman spectroscopic techniques with plasmonic substrates for high temporal resolution, high sensitivity, and high spatial resolution vibrational spectroscopy. First, we introduce background information relevant to ultrafast SERS: the mechanisms of surface enhancement in Raman scattering, the characterization of plasmonic materials with ultrafast techniques, and early complementary techniques to study molecule-plasmon interactions. We then discuss recent advances in surface-enhanced Raman spectroscopies with ultrafast pulses with a focus on the study of molecule-plasmon coupling and molecular dynamics with high sensitivity. We also highlight the challenges faced by this field by the potential damage caused by concentrated, highly energetic pulsed fields in plasmonic hotspots, and finally the potential for future ultrafast SERS studies.

Theoretical Investigation of Device Aspects of Semiconductor Superlattices.

DTIC Science & Technology

1983-09-01

n-i-p-i devices include bulk field effect transistors, ultrasensitive or ultrafast IR photodetectors , tunable light-emitting devices, and ultrafast...transistor4 ultrasensitive or ultrafast IR photodetectors , tunable light-emitt tg devices, and ultrafast optical modulators. Particularlylppealing...differential conductivity ( NDC ) ......................... 19 3.2.2. Spontaneous and stimulated FIR emission from interlayer transitions

A new paradigm for use of ultrafast lasers in ophthalmology for enhancement of corneal mechanical properties and permanent correction of refractive errors

NASA Astrophysics Data System (ADS)

Wang, Chao; Fomovsky, Mikhail; Hall, Jamie R.; Paik, David C.; Trokel, Stephen L.; Vukelic, Sinisa

2017-02-01

A new paradigm for strengthening of corneal tissue as well as permanent correction of refractive errors has been proposed. Ultrafast laser irradiation is confined to the levels below optical breakdown such that tissue damage is avoided while creating an ionization field responsible for subsequent photochemical modification of the stroma. The concept was assed using newly developed platform for precise application of a near-IR femtosecond laser irradiation to the cornea in in-vitro experiments. Targeted irradiation with tightly focused ultrafast laser pulses allows spatially resolved crosslinking in the interior of the porcine cornea in the absence of photosensitizers. The formation of intra- or interstromal covalent bonds in collagen matrix locally increases lamellar density. Due to high resolution, treatment is spatially resolved and therefore can be tailored to either enhance structure of corneal stroma or adjust corneal curvature towards correcting refractive errors. As the induced modification is primarily driven by nonlinear absorption, the treatment is essentially wavelength independent, and as such potentially less harmful than current method of choice, joint application of UVA light irradiation in conjunction with riboflavin. Potential applicability of a near-IR femtosecond laser for biomechanical stabilization of cornea and non-invasive refractive eye corrections is discussed.

Modulation of Crystal Surface and Lattice by Doping: Achieving Ultrafast Metal-Ion Insertion in Anatase TiO2.

PubMed

Wang, Hsin-Yi; Chen, Han-Yi; Hsu, Ying-Ya; Stimming, Ulrich; Chen, Hao Ming; Liu, Bin

2016-10-26

We report that an ultrafast kinetics of reversible metal-ion insertion can be realized in anatase titanium dioxide (TiO 2 ). Niobium ions (Nb 5+ ) were carefully chosen to dope and drive anatase TiO 2 into very thin nanosheets standing perpendicularly onto transparent conductive electrode (TCE) and simultaneously construct TiO 2 with an ion-conducting surface together with expanded ion diffusion channels, which enabled ultrafast metal ions to diffuse across the electrolyte/solid interface and into the bulk of TiO 2 . To demonstrate the superior metal-ion insertion rate, the electrochromic features induced by ion intercalation were examined, which exhibited the best color switching speed of 4.82 s for coloration and 0.91 s for bleaching among all reported nanosized TiO 2 devices. When performed as the anode for the secondary battery, the modified TiO 2 was capable to deliver a highly reversible capacity of 61.2 mAh/g at an ultrahigh specific current rate of 60 C (10.2 A/g). This fast metal-ion insertion behavior was systematically investigated by the well-controlled electrochemical approaches, which quantitatively revealed both the enhanced surface kinetics and bulk ion diffusion rate. Our study could provide a facile methodology to modulate the ion diffusion kinetics for metal oxides.

Ultrafast and Ultrasensitive Gas Sensors Derived from a Large Fermi-Level Shift in the Schottky Junction with Sieve-Layer Modulation.

PubMed

Cheng, Ching-Cheng; Wu, Chia-Lin; Liao, Yu-Ming; Chen, Yang-Fang

2016-07-13

Gas sensors play an important role in numerous fields, covering a wide range of applications, including intelligent systems and detection of harmful and toxic gases. Even though they have attracted much attention, the response time on the order of seconds to minutes is still very slow. To circumvent the existing problems, here, we provide a seminal attempt with the integration of graphene, semiconductor, and an addition sieve layer forming a nanocomposite gas sensor with ultrahigh sensitivity and ultrafast response. The designed sieve layer has a suitable band structure that can serve as a blocking layer to prevent transfer of the charges induced by adsorbed gas molecules into the underlying semiconductor layer. We found that the sensitivity can be reduced to the parts per million level, and the ultrafast response of around 60 ms is unprecedented compared with published graphene-based gas sensors. The achieved high performance can be interpreted well by the large change of the Fermi level of graphene due to its inherent nature of the low density of states and blocking of the sieve layer to prevent charge transfer from graphene to the underlying semiconductor layer. Accordingly, our work is very useful and timely for the development of gas sensors with high performance for practical applications.

CITIUS: An infrared-extreme ultraviolet light source for fundamental and applied ultrafast science

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

Grazioli, C.; Gauthier, D.; Ivanov, R.

2014-02-15

We present the main features of CITIUS, a new light source for ultrafast science, generating tunable, intense, femtosecond pulses in the spectral range from infrared to extreme ultraviolet (XUV). The XUV pulses (about 10{sup 5}-10{sup 8} photons/pulse in the range 14-80 eV) are produced by laser-induced high-order harmonic generation in gas. This radiation is monochromatized by a time-preserving monochromator, also allowing one to work with high-resolution bandwidth selection. The tunable IR-UV pulses (10{sup 12}-10{sup 15} photons/pulse in the range 0.4-5.6 eV) are generated by an optical parametric amplifier, which is driven by a fraction of the same laser pulse thatmore » generates high order harmonics. The IR-UV and XUV pulses follow different optical paths and are eventually recombined on the sample for pump-probe experiments. We also present the results of two pump-probe experiments: with the first one, we fully characterized the temporal duration of harmonic pulses in the time-preserving configuration; with the second one, we demonstrated the possibility of using CITIUS for selective investigation of the ultra-fast dynamics of different elements in a magnetic compound.« less

Multiobjective optimizations of a novel cryocooled dc gun based ultrafast electron diffraction beam line

NASA Astrophysics Data System (ADS)

Gulliford, Colwyn; Bartnik, Adam; Bazarov, Ivan

2016-09-01

We present the results of multiobjective genetic algorithm optimizations of a single-shot ultrafast electron diffraction beam line utilizing a 225 kV dc gun with a novel cryocooled photocathode system and buncher cavity. Optimizations of the transverse projected emittance as a function of bunch charge are presented and discussed in terms of the scaling laws derived in the charge saturation limit. Additionally, optimization of the transverse coherence length as a function of final rms bunch length at the sample location have been performed for three different sample radii: 50, 100, and 200 μ m , for two final bunch charges: 1 05 electrons (16 fC) and 1 06 electrons (160 fC). Example optimal solutions are analyzed, and the effects of disordered induced heating estimated. In particular, a relative coherence length of Lc ,x/σx=0.27 nm /μ m was obtained for a final bunch charge of 1 05 electrons and final bunch length of σt≈100 fs . For a final charge of 1 06 electrons the cryogun produces Lc ,x/σx≈0.1 nm /μ m for σt≈100 - 200 fs and σx≥50 μ m . These results demonstrate the viability of using genetic algorithms in the design and operation of ultrafast electron diffraction beam lines.

From supersonic shear wave imaging to full-field optical coherence shear wave elastography

NASA Astrophysics Data System (ADS)

Nahas, Amir; Tanter, Mickaël; Nguyen, Thu-Mai; Chassot, Jean-Marie; Fink, Mathias; Claude Boccara, A.

2013-12-01

Elasticity maps of tissue have proved to be particularly useful in providing complementary contrast to ultrasonic imaging, e.g., for cancer diagnosis at the millimeter scale. Optical coherence tomography (OCT) offers an endogenous contrast based on singly backscattered optical waves. Adding complementary contrast to OCT images by recording elasticity maps could also be valuable in improving OCT-based diagnosis at the microscopic scale. Static elastography has been successfully coupled with full-field OCT (FF-OCT) in order to realize both micrometer-scale sectioning and elasticity maps. Nevertheless, static elastography presents a number of drawbacks, mainly when stiffness quantification is required. Here, we describe the combination of two methods: transient elastography, based on speed measurements of shear waves induced by ultrasonic radiation forces, and FF-OCT, an en face OCT approach using an incoherent light source. The use of an ultrafast ultrasonic scanner and an ultrafast camera working at 10,000 to 30,000 images/s made it possible to follow shear wave propagation with both modalities. As expected, FF-OCT is found to be much more sensitive than ultrafast ultrasound to tiny shear vibrations (a few nanometers and micrometers, respectively). Stiffness assessed in gel phantoms and an ex vivo rat brain by FF-OCT is found to be in good agreement with ultrasound shear wave elastography.

Diagnostic Performance of Ultrafast Brain MRI for Evaluation of Abusive Head Trauma.

PubMed

Kralik, S F; Yasrebi, M; Supakul, N; Lin, C; Netter, L G; Hicks, R A; Hibbard, R A; Ackerman, L L; Harris, M L; Ho, C Y

2017-04-01

MR imaging with sedation is commonly used to detect intracranial traumatic pathology in the pediatric population. Our purpose was to compare nonsedated ultrafast MR imaging, noncontrast head CT, and standard MR imaging for the detection of intracranial trauma in patients with potential abusive head trauma. A prospective study was performed in 24 pediatric patients who were evaluated for potential abusive head trauma. All patients received noncontrast head CT, ultrafast brain MR imaging without sedation, and standard MR imaging with general anesthesia or an immobilizer, sequentially. Two pediatric neuroradiologists independently reviewed each technique blinded to other modalities for intracranial trauma. We performed interreader agreement and consensus interpretation for standard MR imaging as the criterion standard. Diagnostic accuracy was calculated for ultrafast MR imaging, noncontrast head CT, and combined ultrafast MR imaging and noncontrast head CT. Interreader agreement was moderate for ultrafast MR imaging (κ = 0.42), substantial for noncontrast head CT (κ = 0.63), and nearly perfect for standard MR imaging (κ = 0.86). Forty-two percent of patients had discrepancies between ultrafast MR imaging and standard MR imaging, which included detection of subarachnoid hemorrhage and subdural hemorrhage. Sensitivity, specificity, and positive and negative predictive values were obtained for any traumatic pathology for each examination: ultrafast MR imaging (50%, 100%, 100%, 31%), noncontrast head CT (25%, 100%, 100%, 21%), and a combination of ultrafast MR imaging and noncontrast head CT (60%, 100%, 100%, 33%). Ultrafast MR imaging was more sensitive than noncontrast head CT for the detection of intraparenchymal hemorrhage ( P = .03), and the combination of ultrafast MR imaging and noncontrast head CT was more sensitive than noncontrast head CT alone for intracranial trauma ( P = .02). In abusive head trauma, ultrafast MR imaging, even combined with noncontrast head CT, demonstrated low sensitivity compared with standard MR imaging for intracranial traumatic pathology, which may limit its utility in this patient population. © 2017 by American Journal of Neuroradiology.

Carotid Artery Stiffness Assessment by Ultrafast Ultrasound Imaging: Feasibility and Potential Influencing Factors.

PubMed

Pan, Fu-Shun; Yu, Liang; Luo, Jia; Wu, Ri-Dong; Xu, Ming; Liang, Jin-Yu; Zheng, Yan-Ling; Xie, Xiao-Yan

2018-04-19

To evaluate the feasibility of the ultrafast ultrasound pulsed wave velocity (PWV) for carotid stiffness assessment and potential influencing factors. Ultrafast PWV measurements of 442 carotid arteries in 162 consecutive patients (patient group) and 66 healthy volunteers (control group) were performed. High- and very high-frequency transducers were used in 110 carotid segments. The ultrafast PWVs at the beginning and end of systole were automatically measured. The correlations between the intima-media thickness (IMT) and ultrafast PWV and the equipment and carotid factors influencing the utility of ultrafast PWV were analyzed. Each ultrafast PWV acquisition was completed within 1 minute. The intraobserver variability showed mean differences ± SD of 0.12 ± 1.28 m/s for the PWV before systole and 0.06 ± 1.30 m/s for the PWV at the end of systole. Ultrafast PWV measurements were more likely obtained with the very high- frequency transducer when the IMT was less than 1.5 mm (P < .05). A generalized linear mixed-effects model analysis showed that the very high-frequency transducer had a greater ability to obtain a valid carotid ultrafast PWV measurement with an IMT of less than 1.5 mm (P < .05). The IMT was positively correlated with the PWV before systole and at the end of systole (r = 0.207-0.771; all P < .05) in the control group, patient group, and carotid subgroup with an IMT of less than 1.5 mm. A multiple regression analysis showed that the IMT and plaque were important independent factors in predicting failure of the ultrafast PWV (P < .001). The ultrafast PWV is an effective and user-friendly method for evaluating carotid stiffness. The IMT and transducer type are factors influencing the ability to obtain an ultrafast PWV measurement. © 2018 by the American Institute of Ultrasound in Medicine.

Hot-hole extraction from quantum dot to molecular adsorbate.

PubMed

Singhal, Pallavi; Ghosh, Hirendra N

2015-03-09

Ultrafast thermalized and hot-hole-transfer processes have been investigated in CdSe quantum dot (QD)/catechol composite systems in which hole transfer from photoexcited QDs to the catechols is thermodynamically favorable. A series of catechol derivatives were selected with different electron-donating and -withdrawing groups, and the effect of these groups on hole transfer and charge recombination (CR) dynamics has been investigated. The hole-transfer time was determined using the fluorescence upconversion technique and found to be 2-10 ps depending on the molecular structure of the catechol derivatives. The hot-hole-transfer process was followed after monitoring 2S luminescence of CdSe QDs. Interestingly, hot-hole extraction was observed only in the CdSe/3-methoxycatechol (3-OCH3) composite system owing to the higher electron-donating property of the 3-methoxy group. To confirm the extraction of the hot hole and to monitor the CR reaction in CdSe QD/catechol composite systems, ultrafast transient absorption studies have been carried out. Ultrafast transient-absorption studies show that the bleach recovery kinetics of CdSe QD at the 2S excitonic position is much faster in the presence of 3-OCH3. This faster bleach recovery at the 2S position in CdSe/3-OCH3 suggests hot-hole transfer from CdSe QD to 3-OCH3. CR dynamics in CdSe QD/catechol composite systems was followed by monitoring the excitonic bleach at the 1S position and was found to decrease with free energy of the CR reaction. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales (A "Life at the Frontiers of Energy Research" contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum)

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

None

"The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales" was submitted by the Center for Energy Frontier Research in Extreme Environments (EFree) to the "Life at the Frontiers of Energy Research" video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. EFree is directed by Ho-kwang Mao at the Carnegie Institute of Science in Washington, DC and is a partnership of scientists from thirteen institutions.The Office of Basic Energy Sciences in the U.S. Department of Energy's Office ofmore » Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges. The mission of Energy Frontier Research in Extreme Environments is 'to accelerate the discovery and creation of energy-relevant materials using extreme pressures and temperatures.' Research topics are: catalysis (CO2, water), photocatalysis, solid state lighting, optics, thermelectric, phonons, thermal conductivity, solar electrodes, fuel cells, superconductivity, extreme environment, radiation effects, defects, spin dynamics, CO2 (capture, convert, store), greenhouse gas, hydrogen (fuel, storage), ultrafast physics, novel materials synthesis, and defect tolerant materials.« less

Ultrafast pulse lasers jump to macro applications

NASA Astrophysics Data System (ADS)

Griebel, Martin; Lutze, Walter; Scheller, Torsten

2016-03-01

Ultrafast Lasers have been proven for several micro applications, e.g. stent cutting, for many years. Within its development of applications Jenoptik has started to use ultrafast lasers in macro applications in the automotive industry. The JenLas D2.fs-lasers with power output control via AOM is an ideal tool for closed loop controlled material processing. Jenoptik enhanced his well established sensor controlled laser weakening process for airbag covers to a new level. The patented process enables new materials using this kind of technology. One of the most sensitive cover materials is genuine leather. As a natural product it is extremely inhomogeneous and sensitive for any type of thermal load. The combination of femtosecond pulse ablation and closed loop control by multiple sensor array opens the door to a new quality level of defined weakening. Due to the fact, that the beam is directed by scanning equipment the process can be split in multiple cycles additionally reducing the local energy input. The development used the 5W model as well as the latest 10W release of JenLas D2.fs and achieved amazing processing speeds which directly fulfilled the requirements of the automotive industry. Having in mind that the average cycle time of automotive processes is about 60s, trials had been done of processing weakening lines in genuine leather of 1.2mm thickness. Parameters had been about 15 cycles with 300mm/s respectively resulting in an average speed of 20mm/s and a cycle time even below 60s. First samples had already given into functional and aging tests and passed successfully.

Ultrafast Spectroscopic Noninvasive Probe of Vertical Carrier Transport in Heterostructure Devices

DTIC Science & Technology

2016-03-01

where barriers, tunneling , scattering, strong polarization-induced fields, or carrier localization due to Type I or Type II quantum-well structures can... tunneling across junctions, scattering at heterointerfaces, and internal fields. For light-emitting devices, poor charge transport across multilayer...localization of holes and rapid electron tunneling .5 However, direct transport properties were Approved for public release; distribution is

Near-field infrared vibrational dynamics and tip-enhanced decoherence.

PubMed

Xu, Xiaoji G; Raschke, Markus B

2013-04-10

Ultrafast infrared spectroscopy can reveal the dynamics of vibrational excitations in matter. In its conventional far-field implementation, however, it provides only limited insight into nanoscale sample volumes due to insufficient spatial resolution and sensitivity. Here, we combine scattering-scanning near-field optical microscopy (s-SNOM) with femtosecond infrared vibrational spectroscopy to characterize the coherent vibrational dynamics of a nanoscopic ensemble of C-F vibrational oscillators of polytetrafluoroethylene (PTFE). The near-field mode transfer between the induced vibrational molecular coherence and the metallic scanning probe tip gives rise to a tip-mediated radiative IR emission of the vibrational free-induction decay (FID). By increasing the tip–sample coupling, we can enhance the vibrational dephasing of the induced coherent vibrational polarization and associated IR emission, with dephasing times up to T2(NF) is approximately equal to 370 fs in competition against the intrinsic far-field lifetime of T2(FF) is approximately equal to 680 fs as dominated by nonradiative damping. Near-field antenna-coupling thus provides for a new way to modify vibrational decoherence. This approach of ultrafast s-SNOM enables the investigation of spatiotemporal dynamics and correlations with nanometer spatial and femtosecond temporal resolution.

Ultrafast primary processes of an iron-(III) azido complex in solution induced with 266 nm light.

PubMed

Vennekate, Hendrik; Schwarzer, Dirk; Torres-Alacan, Joel; Krahe, Oliver; Filippou, Alexander C; Neese, Frank; Vöhringer, Peter

2012-05-14

The ultrafast photo-induced primary processes of the iron-(III) azido complex, [Fe(III)N(3)(cyclam-acetato)] PF(6) (1), in acetonitrile solution at room temperature were studied using femtosecond spectroscopy with ultraviolet (UV) excitation and mid-infrared (MIR) detection. Following the absorption of a 266 nm photon, the complex undergoes an internal conversion back to the electronic doublet ground state at a time scale below 2 ps. Subsequently, the electronic ground state vibrationally cools with a characteristic time constant of 13 ps. A homolytic bond cleavage was also observed by the appearance of ground state azide radicals, which were identified by their asymmetric stretching vibration at 1659 cm(-1). The azide radical recombines in a geminate fashion with the iron containing fragment within 20 ps. The cage escape leading to well separated fragments after homolytic Fe-N bond breakage was found to occur with a quantum yield of 35%. Finally, non-geminate recombination at nanosecond time scales was seen to further reduce the photolytic quantum yield to below 20% at a wavelength of 266 nm. This journal is © the Owner Societies 2012

Recombination emissions and spectral blueshift of pump radiation from ultrafast laser induced plasma in a planar water microjet

NASA Astrophysics Data System (ADS)

Anija, M.; Philip, Reji

2009-09-01

We report spectroscopic investigations of an ultrafast laser induced plasma generated in a planar water microjet. Plasma recombination emissions along with the spectral blueshift and broadening of the pump laser pulse contribute to the total emission. The laser pulses are of 100 fs duration, and the incident intensity is around 10 15 W/cm 2. The dominant mechanisms leading to plasma formation are optical tunnel ionization and collisional ionization. Spectrally resolved polarization measurements show that the high frequency region of the emission is unpolarized whereas the low frequency region is polarized. Results indicate that at lower input intensities the emission arises mainly from plasma recombinations, which is accompanied by a weak blueshift of the incident laser pulse. At higher input intensities strong recombination emissions are seen, along with a broadening and asymmetric spectral blueshift of the pump laser pulse. From the nature of the blueshifted laser pulse it is possible to deduce whether the rate of change of free electron density is a constant or variable within the pulse lifetime. Two input laser intensity regimes, in which collisional and tunnel ionizations are dominant respectively, have been thus identified.

Quasi-particles ultrafastly releasing kink bosons to form Fermi arcs in a cuprate superconductor.

PubMed

Ishida, Y; Saitoh, T; Mochiku, T; Nakane, T; Hirata, K; Shin, S

2016-01-05

In a conventional framework, superconductivity is lost at a critical temperature (Tc) because, at higher temperatures, gluing bosons can no longer bind two electrons into a Cooper pair. In high-Tc cuprates, it is still unknown how superconductivity vanishes at Tc. We provide evidence that the so-called ≲ 70-meV kink bosons that dress the quasi-particle excitations are playing a key role in the loss of superconductivity in a cuprate. We irradiated a 170-fs laser pulse on Bi2Sr2CaCu2O(8+δ) and monitored the responses of the superconducting gap and dressed quasi-particles by time- and angle-resolved photoemission spectroscopy. We observe an ultrafast loss of superconducting gap near the d-wave node, or light-induced Fermi arcs, which is accompanied by spectral broadenings and weight redistributions occurring within the kink binding energy. We discuss that the underlying mechanism of the spectral broadening that induce the Fermi arc is the undressing of quasi-particles from the kink bosons. The loss mechanism is beyond the conventional framework, and can accept the unconventional phenomena such as the signatures of Cooper pairs remaining at temperatures above Tc.

Quasi-particles ultrafastly releasing kink bosons to form Fermi arcs in a cuprate superconductor

PubMed Central

Ishida, Y.; Saitoh, T.; Mochiku, T.; Nakane, T.; Hirata, K.; Shin, S.

2016-01-01

In a conventional framework, superconductivity is lost at a critical temperature (Tc) because, at higher temperatures, gluing bosons can no longer bind two electrons into a Cooper pair. In high-Tc cuprates, it is still unknown how superconductivity vanishes at Tc. We provide evidence that the so-called ≲70-meV kink bosons that dress the quasi-particle excitations are playing a key role in the loss of superconductivity in a cuprate. We irradiated a 170-fs laser pulse on Bi2Sr2CaCu2O8+δ and monitored the responses of the superconducting gap and dressed quasi-particles by time- and angle-resolved photoemission spectroscopy. We observe an ultrafast loss of superconducting gap near the d-wave node, or light-induced Fermi arcs, which is accompanied by spectral broadenings and weight redistributions occurring within the kink binding energy. We discuss that the underlying mechanism of the spectral broadening that induce the Fermi arc is the undressing of quasi-particles from the kink bosons. The loss mechanism is beyond the conventional framework, and can accept the unconventional phenomena such as the signatures of Cooper pairs remaining at temperatures above Tc. PMID:26728626

Phonon properties and slow organic-to-inorganic sub-lattice thermalization in hybrid perovskites

NASA Astrophysics Data System (ADS)

Chan, Maria; Chang, Angela; Xia, Yi; Sadasivam, Sridhar; Guo, Peijun; Kinaci, Alper; Lin, Hao-Wu; Darancet, Pierre; Schaller, Richard

Organic-inorganic hybrid perovskite halide compounds have been investigated extensively for photovoltaics (PVs) and related applications. The thermal transport properties of hybrid perovskites, including phonon-carrier and phonon-phonon interactions, are of significance for their PV and solar thermoelectric applications. The interlocking organic and inorganic sublattices can be thought of as an extreme form of nanostructuring. A result of this nanostructuring is the large gap in phonon frequencies between the organic and inorganic sublattices, which is expected to create bottlenecks in phonon equilibration. In this work, we use a combination of ultrafast spectroscopy including photoluminescence and transient absorption, as well as first principles density functional theory (DFT), ab initio molecular dynamics calculations, phonon lifetimes derived from DFT force constants, and non-equilibrium phonon dynamics accounting for phonon lifetimes, to determine the phonon and charge interaction processes. We find evidence that thermalization of carriers occur at an atypically slow 50-100 ps time scale owing to the complex interplay between electronic and phonon excitations.

Multifunctional non-woven fabrics of interfused graphene fibres

PubMed Central

Li, Zheng; Xu, Zhen; Liu, Yingjun; Wang, Ran; Gao, Chao

2016-01-01

Carbon-based fibres hold promise for preparing multifunctional fabrics with electrical conductivity, thermal conductivity, permeability, flexibility and lightweight. However, these fabrics are of limited performance mainly because of the weak interaction between fibres. Here we report non-woven graphene fibre fabrics composed of randomly oriented and interfused graphene fibres with strong interfibre bonding. The all-graphene fabrics obtained through a wet-fusing assembly approach are porous and lightweight, showing high in-plane electrical conductivity up to ∼2.8 × 104 S m−1 and prominent thermal conductivity of ∼301.5 W m−1 K−1. Given the low density (0.22 g cm−3), their specific electrical and thermal conductivities set new records for carbon-based papers/fabrics and even surpass those of individual graphene fibres. The as-prepared fabrics are further used as ultrafast responding electrothermal heaters and durable oil-adsorbing felts, demonstrating their great potential as high-performance and multifunctional fabrics in real-world applications. PMID:27901022

Thermal and Kerr nonlinear properties of plasma-deposited silicon nitride/ silicon dioxide waveguides.

PubMed

Ikeda, Kazuhiro; Saperstein, Robert E; Alic, Nikola; Fainman, Yeshaiahu

2008-08-18

We introduce and present experimental evaluations of loss and nonlinear optical response in a waveguide and an optical resonator, both implemented with a silicon nitride/ silicon dioxide material platform prepared by plasma-enhanced chemical vapor deposition with dual frequency reactors that significantly reduce the stress and the consequent loss of the devices. We measure a relatively small loss of approximately 4dB/cm in the waveguides. The fabricated ring resonators in add-drop and all-pass arrangements demonstrate quality factors of Q=12,900 and 35,600. The resonators are used to measure both the thermal and ultrafast Kerr nonlinearities. The measured thermal nonlinearity is larger than expected, which is attributed to slower heat dissipation in the plasma-deposited silicon dioxide film. The n2 for silicon nitride that is unknown in the literature is measured, for the first time, as 2.4 x 10(-15)cm(2)/W, which is 10 times larger than that for silicon dioxide.

Precision resection of intestine using ultrashort laser pulses

NASA Astrophysics Data System (ADS)

Beck, Rainer J.; Gora, Wojciech S.; Jayne, David; Hand, Duncan P.; Shephard, Jonathan D.

2016-03-01

Endoscopic resection of early colorectal neoplasms typically employs electrocautery tools, which lack precision and run the risk of full thickness thermal injury to the bowel wall with subsequent perforation. We present a means of endoluminal colonic ablation using picosecond laser pulses as a potential alternative to mitigate these limitations. High intensity ultrashort laser pulses enable nonlinear absorption processes, plasma generation, and as a consequence a predominantly non-thermal ablation regimen. Robust process parameters for the laser resection are demonstrated using fresh ex vivo pig intestine samples. Square cavities with comparable thickness to early colorectal neoplasms are removed for a wavelength of 1030 nm and 515 nm using a picosecond laser system. The corresponding histology sections exhibit in both cases only minimal collateral damage to the surrounding tissue. The ablation depth can be controlled precisely by means of the pulse energy. Overall, the application of ultrafast lasers for the resection of intestine enables significantly improved precision and reduced thermal damage to the surrounding tissue compared to conventional electrocautery.

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. Counterintuitively, singlet excited-state lifetime increases on going from Cl (85 fs) to Br (128 fs) and to I (152 fs). Moreover, correlation between the Re-X stretching mode and the rate of ISC is observed. In this Account, we emphasize on the role of spin-vibronic coupling on the mechanism of ultrafast ISC put in evidence in [Re(Br)(CO)3(bpy)]. For this purpose, we have developed a model Hamiltonian for solving an 11 electronic excited states multimode problem including vibronic and SO coupling within the linear vibronic coupling (LVC) approximation and the assumption of harmonic potentials. The presence of a central metal atom coupled to rigid ligands, such as α-diimine, ensures nuclear motion of small amplitudes and a priori justifies the use of the LVC model. The simulation of the ultrafast dynamics by wavepacket propagations using the multiconfiguration time-dependent Hartree (MCTDH) method is based on density functional theory (DFT), and its time-dependent extension to excited states (TD-DFT) electronic structure data. We believe that the interplay between time-resolved experiments and these pioneering simulations covering the first picoseconds and including spin-vibronic coupling will promote a number of quantum dynamical studies that will contribute to a better understanding of ultrafast processes in a wide range of organic and inorganic chromophores easily incorporated in biosystems or supramolecular devices for specific functions.

Shock Induced Chemistry: Application and Development of Ultrafast Nonlinear Probes of the Energy Dynamics of Molecules in Solids

DTIC Science & Technology

1988-01-01

crystal and in a mixed crystal. The mixed crystal data was taken with resonance enhancement by the pentacene .. ... 7 Accesiw, r)re 0IE r)) NiS cR4~ IE~) D...observations as well as their implications about the nature of the coupling of a localized defect to the bulk modes of the crystal have been analyzed [7...matter systems, in addition to phonon induced fluctuations of local mechanical properties, there can be much slower timescale structural evolution

In Situ Localized Growth of Ordered Metal Oxide Hollow Sphere Array on Microheater Platform for Sensitive, Ultra-Fast Gas Sensing.

PubMed

Rao, Ameya; Long, Hu; Harley-Trochimczyk, Anna; Pham, Thang; Zettl, Alex; Carraro, Carlo; Maboudian, Roya

2017-01-25

A simple and versatile strategy is presented for the localized on-chip synthesis of an ordered metal oxide hollow sphere array directly on a low power microheater platform to form a closely integrated miniaturized gas sensor. Selective microheater surface modification through fluorinated monolayer self-assembly and its subsequent microheater-induced thermal decomposition enables the position-controlled deposition of an ordered two-dimensional colloidal sphere array, which serves as a sacrificial template for metal oxide growth via homogeneous chemical precipitation; this strategy ensures control in both the morphology and placement of the sensing material on only the active heated area of the microheater platform, providing a major advantage over other methods of presynthesized nanomaterial integration via suspension coating or printing. A fabricated tin oxide hollow sphere-based sensor shows high sensitivity (6.5 ppb detection limit) and selectivity toward formaldehyde, and extremely fast response (1.8 s) and recovery (5.4 s) times. This flexible and scalable method can be used to fabricate high performance miniaturized gas sensors with a variety of hollow nanostructured metal oxides for a range of applications, including combining multiple metal oxides for superior sensitivity and tunable selectivity.

Extreme ultraviolet probing of nonequilibrium dynamics in high energy density germanium

NASA Astrophysics Data System (ADS)

Principi, E.; Giangrisostomi, E.; Mincigrucci, R.; Beye, M.; Kurdi, G.; Cucini, R.; Gessini, A.; Bencivenga, F.; Masciovecchio, C.

2018-05-01

Intense femtosecond infrared laser pulses induce a nonequilibrium between thousands of Kelvin hot valence electrons and room-temperature ions in a germanium sample foil. The evolution of this exotic state of matter is monitored with time-resolved extreme ultraviolet absorption spectroscopy across the Ge M2 ,3 edge (≃30 eV ) using the FERMI free-electron laser. We analyze two distinct regimes in the ultrafast dynamics in laser-excited Ge: First, on a subpicosecond time scale, the electron energy distribution thermalizes to an extreme temperature unreachable in equilibrium solid germanium; then, during the following picoseconds, the lattice reacts strongly altering the electronic structure and resulting in melting to a metallic state alongside a breakdown of the local atomic order. Data analysis, based on a hybrid approach including both numerical and analytical calculations, provides an estimation of the electron and ion temperatures, the electron density of states, the carrier-phonon relaxation time, as well as the carrier density and lattice heat capacity under those extreme nonequilibrium conditions. Related structural anomalies, such as the occurrence of a transient low-density liquid phase and the possible drop in lattice heat capacity are discussed.

Control of dynamical self-assembly of strongly Brownian nanoparticles through convective forces induced by ultrafast laser

NASA Astrophysics Data System (ADS)

Ilday, Serim; Akguc, Gursoy B.; Tokel, Onur; Makey, Ghaith; Yavuz, Ozgun; Yavuz, Koray; Pavlov, Ihor; Ilday, F. Omer; Gulseren, Oguz

We report a new dynamical self-assembly mechanism, where judicious use of convective and strong Brownian forces enables effective patterning of colloidal nanoparticles that are almost two orders of magnitude smaller than the laser beam. Optical trapping or tweezing effects are not involved, but the laser is used to create steep thermal gradients through multi-photon absorption, and thereby guide the colloids through convective forces. Convective forces can be thought as a positive feedback mechanism that helps to form and reinforce pattern, while Brownian motion act as a competing negative feedback mechanism to limit the growth of the pattern, as well as to increase the possibilities of bifurcation into different patterns, analogous to the competition observed in reaction-diffusion systems. By steering stochastic processes through these forces, we are able to gain control over the emergent pattern such as to form-deform-reform of a pattern, to change its shape and transport it spatially within seconds. This enables us to dynamically initiate and control large patterns comprised of hundreds of colloids. Further, by not relying on any specific chemical, optical or magnetic interaction, this new method is, in principle, completely independent of the material type being assembled.

Enhanced Evaporation Strength through Fast Water Permeation in Graphene-Oxide Deposition

PubMed Central

Li Tong, Wei; Ong, Wee-Jun; Chai, Siang-Piao; Tan, Ming K.; Mun Hung, Yew

2015-01-01

The unique characteristic of fast water permeation in laminated graphene oxide (GO) sheets has facilitated the development of ultrathin and ultrafast nanofiltration membranes. Here we report the application of fast water permeation property of immersed GO deposition for enhancing the performance of a GO/water nanofluid charged two-phase closed thermosyphon (TPCT). By benchmarking its performance against a silver oxide/water nanofluid charged TPCT, the enhancement of evaporation strength is found to be essentially attributed to the fast water permeation property of GO deposition instead of the enhanced surface wettability of the deposited layer. The expansion of interlayer distance between the graphitic planes of GO deposited layer enables intercalation of bilayer water for fast water permeation. The capillary force attributed to the frictionless interaction between the atomically smooth, hydrophobic carbon structures and the well-ordered hydrogen bonds of water molecules is sufficiently strong to overcome the gravitational force. As a result, a thin water film is formed on the GO deposited layers, inducing filmwise evaporation which is more effective than its interfacial counterpart, appreciably enhanced the overall performance of TPCT. This study paves the way for a promising start of employing the fast water permeation property of GO in thermal applications. PMID:26100977

Ultrafast proton radiography of the magnetic fields generated by a laser-driven coil current

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

Gao, Lan; Ji, Hantao; Princeton Plasma Physics Laboratory, Princeton University, Princeton, New Jersey 08543

2016-04-15

Magnetic fields generated by a current flowing through a U-shaped coil connecting two copper foils were measured using ultrafast proton radiography. Two ∼1.25 kJ, 1-ns laser pulses propagated through laser entrance holes in the front foil and were focused to the back foil with an intensity of ∼3 × 10{sup 16 }W/cm{sup 2}. The intense laser-solid interaction induced a high voltage between the copper foils and generated a large current in the connecting coil. The proton data show ∼40–50 T magnetic fields at the center of the coil ∼3–4 ns after laser irradiation. The experiments provide significant insight for future target designs that aim tomore » develop a powerful source of external magnetic fields for various applications in high-energy-density science.« less

Through-Space Ultrafast Photoinduced Electron Transfer Dynamics of a C 70 -Encapsulated Bisporphyrin Covalent Organic Polyhedron in a Low-Dielectric Medium

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

Ortiz, Michael; Cho, Sung; Niklas, Jens

Ultrafast photoinduced electron transfer (PIET) dynamics of a C 70-encapsulated bisporphyrin covalent organic polyhedron hybrid (C 70@COP-5) is studied in a nonpolar toluene medium with fluorescence and transient absorption spectroscopies. This structurally rigid donor (D)-acceptor (A) molecular hybrid offers a new platform featuring conformationally predetermined cofacial D-A orientation with a fixed edge-to-edge separation, R EE (2.8 Å), without the aid of covalent bonds. Sub-picosecond PIET (T ET ≤ 0.4 ps) and very slow charge recombination (T CR ≈ 600 ps) dynamics are observed. The origin of these dynamics is discussed in terms of enhanced D-A coupling (V = 675 cmmore » -1) and extremely small reorganization energy (λ ≈ 0.18 eV), induced by the intrinsic structural rigidity of the C 70@COP-5 complex.« less

Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase.

PubMed

Lu, Jian; Zhang, Yaqing; Hwang, Harold Y; Ofori-Okai, Benjamin K; Fleischer, Sharly; Nelson, Keith A

2016-10-18

Ultrafast 2D spectroscopy uses correlated multiple light-matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum; its extension to the terahertz regime of the electromagnetic spectrum, where a rich variety of material degrees of freedom reside, remains an experimental challenge. We report a demonstration of ultrafast 2D terahertz spectroscopy of gas-phase molecular rotors at room temperature. Using time-delayed terahertz pulse pairs, we observe photon echoes and other nonlinear signals resulting from molecular dipole orientation induced by multiple terahertz field-dipole interactions. The nonlinear time domain orientation signals are mapped into the frequency domain in 2D rotational spectra that reveal J-state-resolved nonlinear rotational dynamics. The approach enables direct observation of correlated rotational transitions and may reveal rotational coupling and relaxation pathways in the ground electronic and vibrational state.

Through-Space Ultrafast Photoinduced Electron Transfer Dynamics of a C 70 -Encapsulated Bisporphyrin Covalent Organic Polyhedron in a Low-Dielectric Medium

DOE PAGES

Ortiz, Michael; Cho, Sung; Niklas, Jens; ...

2017-03-13

Ultrafast photoinduced electron transfer (PIET) dynamics of a C 70-encapsulated bisporphyrin covalent organic polyhedron hybrid (C 70@COP-5) is studied in a nonpolar toluene medium with fluorescence and transient absorption spectroscopies. This structurally rigid donor (D)-acceptor (A) molecular hybrid offers a new platform featuring conformationally predetermined cofacial D-A orientation with a fixed edge-to-edge separation, R EE (2.8 Å), without the aid of covalent bonds. Sub-picosecond PIET (T ET ≤ 0.4 ps) and very slow charge recombination (T CR ≈ 600 ps) dynamics are observed. The origin of these dynamics is discussed in terms of enhanced D-A coupling (V = 675 cmmore » -1) and extremely small reorganization energy (λ ≈ 0.18 eV), induced by the intrinsic structural rigidity of the C 70@COP-5 complex.« less

Through-Space Ultrafast Photoinduced Electron Transfer Dynamics of a C70-Encapsulated Bisporphyrin Covalent Organic Polyhedron in a Low-Dielectric Medium.

PubMed

Ortiz, Michael; Cho, Sung; Niklas, Jens; Kim, Seonah; Poluektov, Oleg G; Zhang, Wei; Rumbles, Garry; Park, Jaehong

2017-03-29

Ultrafast photoinduced electron transfer (PIET) dynamics of a C 70 -encapsulated bisporphyrin covalent organic polyhedron hybrid (C 70 @COP-5) is studied in a nonpolar toluene medium with fluorescence and transient absorption spectroscopies. This structurally rigid donor (D)-acceptor (A) molecular hybrid offers a new platform featuring conformationally predetermined cofacial D-A orientation with a fixed edge-to-edge separation, R EE (2.8 Å), without the aid of covalent bonds. Sub-picosecond PIET (τ ET ≤ 0.4 ps) and very slow charge recombination (τ CR ≈ 600 ps) dynamics are observed. The origin of these dynamics is discussed in terms of enhanced D-A coupling (V = 675 cm -1 ) and extremely small reorganization energy (λ ≈ 0.18 eV), induced by the intrinsic structural rigidity of the C 70 @COP-5 complex.

Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface

DOE PAGES

Forst, M.; Wilkins, S. B.; Caviglia, A. D.; ...

2015-07-06

Static strain in complex oxide heterostructures 1,2 has been extensively used to engineer electronic and magnetic properties at equilibrium 3. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across heterointerfaces dynamically 4. Here, by exciting large-amplitude infrared-active vibrations in a LaAlO 3 substrate we induce magnetic order melting in a NdNiO 3 film across a heterointerface. Femtosecond resonant soft X-ray diffraction is used to determine the spatiotemporal evolution of the magnetic disordering. We observe a magnetic melt front that propagates from the substrate interface into the film, at a speedmore » that suggests electronically driven motion. Lastly, light control and ultrafast phase front propagation at heterointerfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.« less

Tracking the coherent generation of polaron pairs in conjugated polymers

NASA Astrophysics Data System (ADS)

de Sio, Antonietta; Troiani, Filippo; Maiuri, Margherita; Réhault, Julien; Sommer, Ephraim; Lim, James; Huelga, Susana F.; Plenio, Martin B.; Rozzi, Carlo Andrea; Cerullo, Giulio; Molinari, Elisa; Lienau, Christoph

2016-12-01

The optical excitation of organic semiconductors not only generates charge-neutral electron-hole pairs (excitons), but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence at room temperature. The measured two-dimensional spectra show pronounced peak splittings revealing that the elementary optical excitations of this polymer are hybridized exciton-polaron-pairs, strongly coupled to a dominant underdamped vibrational mode. Coherent vibronic coupling induces ultrafast polaron pair formation, accelerates the charge separation dynamics and makes it insensitive to disorder. These findings open up new perspectives for tailoring light-to-current conversion in organic materials.

New developments in ophthalmic applications of ultrafast lasers

NASA Astrophysics Data System (ADS)

Spooner, Greg J. R.; Juhasz, Tibor; Ratkay-Traub, Imola; Djotyan, Gagik P.; Horvath, Christopher; Sacks, Zachary S.; Marre, Gabrielle; Miller, Doug L.; Williams, A. R.; Kurtz, Ron M.

2000-05-01

The eye is potentially an ideal target for high precision surgical procedures utilizing ultrafast lasers. We present progress on corneal applications now being tested in humans and proof of concept ex vivo demonstrations of new applications in the sclera and lens. Two corneal refractive procedures were tested in partially sighted human eyes: creation of corneal flaps prior to excimer ablation (Femto- LASIK) and creation of corneal channels and entry cuts for placement of intracorneal ring segments (Femto-ICRS). For both procedures, results were comparable to standard treatments, with the potential for improved safety, accuracy and reproducibility. For scleral applications, we evaluated the potential of femtosecond laser glaucoma surgery by demonstrating resections in ex vivo human sclera using dehydrating agents to induce tissue transparency. For lens applications, we demonstrate in an ex vivo model the use of photodisruptively-nucleated ultrasonic cavitation for local and non-invasive tissue interaction.

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

NASA Astrophysics Data System (ADS)

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

2017-01-01

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

Ultrafast dynamics of multi-exciton state coupled to coherent vibration in zinc chlorin aggregates for artificial photosynthesis.

PubMed

Shi, Tongchao; Liu, Zhengzheng; Miyatake, Tomohiro; Tamiaki, Hitoshi; Kobayashi, Takayoshi; Zhang, Zeyu; Du, Juan; Leng, Yuxin

2017-11-27

Ultrafast vibronic dynamics induced by the interaction of the Frenkel exciton with the coherent molecular vibrations in a layer-structured zinc chlorin aggregates prepared for artificial photosynthesis have been studied by 7.1 fs real-time vibrational spectroscopy with multi-spectrum detection. The fast decay of 100 ± 5fs is ascribed to the relaxation from the higher multi-exciton state (MES) to the one-exciton state, and the slow one of 863 ± 70fs is assigned to the relaxation from Q-exciton state to the dark nonfluorescent charge-transfer (CT) state, respectively. In addition, the wavelength dependences of the exciton-vibration coupling strength are found to follow the zeroth derivative of the transient absorption spectra of the exciton. It could be explained in term of the transition dipole moment modulated by dynamic intensity borrowing between the B transition and the Q transition through the vibronic interactions.

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.

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

Ultrafast coherent excitation of a trapped ion qubit for fast gates and photon frequency qubits.

PubMed

Madsen, M J; Moehring, D L; Maunz, P; Kohn, R N; Duan, L-M; Monroe, C

2006-07-28

We demonstrate ultrafast coherent excitation of an atomic qubit stored in the hyperfine levels of a single trapped cadmium ion. Such ultrafast excitation is crucial for entangling networks of remotely located trapped ions through the interference of photon frequency qubits, and is also a key component for realizing ultrafast quantum gates between Coulomb-coupled ions.

Impact and recovery process of mini flash crashes: An empirical study.

PubMed

Braun, Tobias; Fiegen, Jonas A; Wagner, Daniel C; Krause, Sebastian M; Guhr, Thomas

2018-01-01

In an Ultrafast Extreme Event (or Mini Flash Crash), the price of a traded stock increases or decreases strongly within milliseconds. We present a detailed study of Ultrafast Extreme Events in stock market data. In contrast to popular belief, our analysis suggests that most of the Ultrafast Extreme Events are not necessarily due to feedbacks in High Frequency Trading: In at least 60 percent of the observed Ultrafast Extreme Events, the largest fraction of the price change is due to a single market order. In times of financial crisis, large market orders are more likely which leads to a significant increase of Ultrafast Extreme Events occurrences. Furthermore, we analyze the 100 trades following each Ultrafast Extreme Events. While we observe a tendency of the prices to partially recover, less than 40 percent recover completely. On the other hand we find 25 percent of the Ultrafast Extreme Events to be almost recovered after only one trade which differs from the usually found price impact of market orders.

Impact and recovery process of mini flash crashes: An empirical study

PubMed Central

Wagner, Daniel C.; Krause, Sebastian M.; Guhr, Thomas

2018-01-01

In an Ultrafast Extreme Event (or Mini Flash Crash), the price of a traded stock increases or decreases strongly within milliseconds. We present a detailed study of Ultrafast Extreme Events in stock market data. In contrast to popular belief, our analysis suggests that most of the Ultrafast Extreme Events are not necessarily due to feedbacks in High Frequency Trading: In at least 60 percent of the observed Ultrafast Extreme Events, the largest fraction of the price change is due to a single market order. In times of financial crisis, large market orders are more likely which leads to a significant increase of Ultrafast Extreme Events occurrences. Furthermore, we analyze the 100 trades following each Ultrafast Extreme Events. While we observe a tendency of the prices to partially recover, less than 40 percent recover completely. On the other hand we find 25 percent of the Ultrafast Extreme Events to be almost recovered after only one trade which differs from the usually found price impact of market orders. PMID:29782503

Hydration-reduced lattice thermal conductivity of olivine in Earth's upper mantle.

PubMed

Chang, Yun-Yuan; Hsieh, Wen-Pin; Tan, Eh; Chen, Jiuhua

2017-04-18

Earth's water cycle enables the incorporation of water (hydration) in mantle minerals that can influence the physical properties of the mantle. Lattice thermal conductivity of mantle minerals is critical for controlling the temperature profile and dynamics of the mantle and subducting slabs. However, the effect of hydration on lattice thermal conductivity remains poorly understood and has often been assumed to be negligible. Here we have precisely measured the lattice thermal conductivity of hydrous San Carlos olivine (Mg 0.9 Fe 0.1 ) 2 SiO 4 (Fo90) up to 15 gigapascals using an ultrafast optical pump-probe technique. The thermal conductivity of hydrous Fo90 with ∼7,000 wt ppm water is significantly suppressed at pressures above ∼5 gigapascals, and is approximately 2 times smaller than the nominally anhydrous Fo90 at mantle transition zone pressures, demonstrating the critical influence of hydration on the lattice thermal conductivity of olivine in this region. Modeling the thermal structure of a subducting slab with our results shows that the hydration-reduced thermal conductivity in hydrated oceanic crust further decreases the temperature at the cold, dry center of the subducting slab. Therefore, the olivine-wadsleyite transformation rate in the slab with hydrated oceanic crust is much slower than that with dry oceanic crust after the slab sinks into the transition zone, extending the metastable olivine to a greater depth. The hydration-reduced thermal conductivity could enable hydrous minerals to survive in deeper mantle and enhance water transportation to the transition zone.

Noninvasive Imaging of the Coronary Vasculature Using Ultrafast Ultrasound.

PubMed

Maresca, David; Correia, Mafalda; Villemain, Olivier; Bizé, Alain; Sambin, Lucien; Tanter, Mickael; Ghaleh, Bijan; Pernot, Mathieu

2017-08-11

The aim of this study was to investigate the potential of coronary ultrafast Doppler angiography (CUDA), a novel vascular imaging technique based on ultrafast ultrasound, to image noninvasively with high sensitivity the intramyocardial coronary vasculature and quantify the coronary blood flow dynamics. Noninvasive coronary imaging techniques are currently limited to the observation of the epicardial coronary arteries. However, many studies have highlighted the importance of the coronary microcirculation and microvascular disease. CUDA was performed in vivo in open-chest procedures in 9 swine. Ultrafast plane-wave imaging at 2,000 frames/s was combined to an adaptive spatiotemporal filtering to achieve ultrahigh-sensitive imaging of the coronary blood flows. Quantification of the flow change was performed during hyperemia after a 30-s left anterior descending (LAD) artery occlusion followed by reperfusion and was compared to gold standard measurements provided by a flowmeter probe placed at a proximal location on the LAD (n = 5). Coronary flow reserve was assessed during intravenous perfusion of adenosine. Vascular damages were evaluated during a second set of experiments in which the LAD was occluded for 90 min, followed by 150 min of reperfusion to induce myocardial infarction (n = 3). Finally, the transthoracic feasibility of CUDA was assessed on 2 adult and 2 pediatric volunteers. Ultrahigh-sensitive cine loops of venous and arterial intramyocardial blood flows were obtained within 1 cardiac cycle. Quantification of the coronary flow changes during hyperemia was in good agreement with gold standard measurements (r 2  = 0.89), as well as the assessment of coronary flow reserve (2.35 ± 0.65 vs. 2.28 ± 0.84; p = NS). On the infarcted animals, CUDA images revealed the presence of strong hyperemia and the appearance of abnormal coronary vessel structures in the reperfused LAD territory. Finally, the feasibility of transthoracic coronary vasculature imaging was shown on 4 human volunteers. Ultrafast Doppler imaging can map the coronary vasculature with high sensitivity and quantify intramural coronary blood flow changes. Copyright © 2017 The Authors. Published by Elsevier Inc. All rights reserved.

Ultrafast laser-induced modifications of energy bands of non-metal crystals

NASA Astrophysics Data System (ADS)

Gruzdev, Vitaly

2009-10-01

Ultrafast laser-induced variations of electron energy bands of transparent solids significantly influence ionization and conduction-band electron absorption driving the initial stage of laser-induced damage (LID). The mechanisms of the variations are attributed to changing electron functions from bonding to anti-bonding configuration via laser-induced ionization; laser-driven electron oscillations in quasi-momentum space; and direct distortion of the inter-atomic potential by electric field of laser radiation. The ionization results in the band-structure modification via accumulation of broken chemical bonds between atoms and provides significant contribution to the overall modification only when enough excited electrons are accumulated in the conduction band. The oscillations are associated with modification of electron energy by pondermotive potential of the oscillations. The direct action of radiation's electric field leads to specific high-frequency Franz-Keldysh effect (FKE) spreading the allowed electron states into the bands of forbidden energy. Those processes determine the effective band gap that is a laser-driven energy gap between the modified electron energy bands. Among those mechanisms, the latter two provide reversible band-structure modification that takes place from the beginning of the ionization and are, therefore, of special interest due to their strong influence on the initial stage of the ionization. The pondermotive potential results either in monotonous increase or oscillatory variations of the effective band gap that has been taken into account in some ionization models. The classical FKE provides decrease of the band gap. We analyzing the competition between those two opposite trends of the effective-band-gap variations and discuss applications of those effects for considerations of the laser-induced damage and its threshold in transparent solids.

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-infrared excitation. With the help of the field enhancement in metamaterial split ring resonator gaps, we obtain picosecond THz electric field transients of several MV/cm which is sufficient to drive the insulator to metal transition in V02.

Ultrafast Silicon-based Modulators using Optical Switching of Vanadium Dioxide

DTIC Science & Technology

2014-12-04

demonstrated by using photothermal heating to induce the VO2 semiconductor-to- metal phase transition and modulate the transmitted optical signal...speeds. By utilizing the sub-picosecond semiconductor-to- metal transition (SMT) in VO2 as the active switching mechanism that enables direct... metallic phases. The steep slope, high contrast, and relatively narrow hysteresis exhibited by these reflectivity measurements indicate the high quality

Femtosecond tracking of carrier relaxation in germanium with extreme ultraviolet transient reflectivity

NASA Astrophysics Data System (ADS)

Kaplan, Christopher J.; Kraus, Peter M.; Ross, Andrew D.; Zürch, Michael; Cushing, Scott K.; Jager, Marieke F.; Chang, Hung-Tzu; Gullikson, Eric M.; Neumark, Daniel M.; Leone, Stephen R.

2018-05-01

Extreme ultraviolet (XUV) transient reflectivity around the germanium M4 ,5 edge (3 d core-level to valence transition) at 30 eV is advanced to obtain the transient dielectric function of crystalline germanium [100] on femtosecond to picosecond time scales following photoexcitation by broadband visible-to-infrared (VIS/NIR) pulses. By fitting the transient dielectric function, carrier-phonon induced relaxations are extracted for the excited carrier distribution. The measurements reveal a hot electron relaxation rate of 3.2 ±0.2 ps attributed to the X -L intervalley scattering and a hot hole relaxation rate of 600 ±300 fs ascribed to intravalley scattering within the heavy hole (HH) band, both in good agreement with previous work. An overall energy shift of the XUV dielectric function is assigned to a thermally induced band gap shrinkage by formation of acoustic phonons, which is observed to be on a timescale of 4-5 ps, in agreement with previously measured optical phonon lifetimes. The results reveal that the transient reflectivity signal at an angle of 66∘ with respect to the surface normal is dominated by changes to the real part of the dielectric function, due to the near critical angle of incidence of the experiment (66∘-70∘) for the range of XUV energies used. This work provides a methodology for interpreting XUV transient reflectivity near core-level transitions, and it demonstrates the power of the XUV spectral region for measuring ultrafast excitation dynamics in solids.

Ultrafast Nonlinear Response of Atomic and Molecular Gases in Near-IR and Mid-IR Regions

NASA Astrophysics Data System (ADS)

Zahedpour Anaraki, Sina

There is a dynamical interaction between an ultrashort laser pulse and the medium it propagates through. At the shortest timescales, the near-instantaneous electronic response of the medium contributes to an induced polarization nonlinearity. On a longer timescale, the vibrational response can contribute, followed on even longer timescales by the rotational response. One of the major consequences of these nonlinearities is that they can induce the collapse and filamentation of the laser pulse, leading to ionization and plasma generation. In this dissertation, measurements and theory are presented for both the fundamental atomic and molecular nonlinearities themselves (electronic, rovibrational, and ionization rates) in the range lambda=400nm-2600nm, and their applications. The media investigated are air constituents (Ar, N 2, O2), H2, D2, and common transparent optical materials. In particular, in one application it is shown that in molecular gases like N2 and O2, the propagating laser electric field can pump a rotational wavepacket, producing molecular ensembles with both transient and long-lived ("permanent") alignment components. This alignment, which generates quantum echoes (rotational revivals), can interact with the pulse that generated it (rotational nonlinearity) and with any pulses that may follow. We show that a properly timed train of ultrashort laser pulses can resonate with the rotational revivals, causing a "permanent" alignment in the gas which thermalizes and then drives a strong hydrodynamic response which can exceed that from the plasma heating by a filament.

Ultrafast Spectroscopy of Proton-Coupled Electron Transfer (PCET) in Photocatalysis

DTIC Science & Technology

2016-07-08

AFRL-AFOSR-VA-TR-2016-0244 Ultrafast Spectroscopy of Proton-Coupled Electron Transfer (PCET) in Photocatalysis Jahan Dawlaty UNIVERSITY OF SOUTHERN...TITLE AND SUBTITLE Ultrafast Spectroscopy of Proton-Coupled Electron Transfer (PCET) in Photocatalysis 5a. CONTRACT NUMBER 5b. GRANT NUMBER FA9550...298 Back (Rev. 8/98) DISTRIBUTION A: Distribution approved for public release. Final Report: AFOSR YIP Grant FA9550-13-1-0128: Ultrafast Spectroscopy

Feasibility of UltraFast Doppler in Post-operative Evaluation of Hepatic Artery in Recipients following Liver Transplantation.

PubMed

Kim, Se-Young; Kim, Kyoung Won; Choi, Sang Hyun; Kwon, Jae Hyun; Song, Gi-Won; Kwon, Heon-Ju; Yun, Young Ju; Lee, Jeongjin; Lee, Sung-Gyu

2017-11-01

To determine the feasibility of using UltraFast Doppler in post-operative evaluation of the hepatic artery (HA) after liver transplantation (LT), we evaluated 283 simultaneous conventional and UltraFast Doppler sessions in 126 recipients over a 2-mo period after LT, using an Aixplorer scanner The Doppler indexes of the HA (peak systolic velocity [PSV], end-diastolic velocity [EDV], resistive index [RI] and systolic acceleration time [SAT]) by retrospective analysis of retrieved waves from UltraFast Doppler clips were compared with those obtained by conventional spectral Doppler. Correlation, performance in diagnosing the pathologic wave, examination time and reproducibility were evaluated. The PSV, EDV, RI and SAT of spectral and UltraFast Doppler measurements exhibited excellent correlation with favorable diagnostic performance. During the bedside examination, the mean time spent for UltraFast clip storing was significantly shorter than that for conventional Doppler US measurements. Both conventional and UltraFast Doppler exhibited good to excellent inter-analysis consistency. In conclusion, compared with conventional spectral Doppler, UltraFast Doppler values correlated excellently and yielded acceptable pathologic wave diagnostic performance with reduced examination time at the bedside and excellent reproducibility. Copyright © 2017 World Federation for Ultrasound in Medicine & Biology. Published by Elsevier Inc. All rights reserved.

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.

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.

Near atomically smooth alkali antimonide photocathode thin films

DOE PAGES

Feng, Jun; Karkare, Siddharth; Nasiatka, James; ...

2017-01-24

Nano-roughness is one of the major factors degrading the emittance of electron beams that can be generated by high efficiency photocathodes, such as the thermally reacted alkali antimonide thin films. In this paper, we demonstrate a co-deposition based method for producing alkali antimonide cathodes that produce near atomic smoothness with high reproducibility. Here, we calculate the effect of the surface roughness on the emittance and show that such smooth cathode surfaces are essential for operation of alkali antimonide cathodes in high field, low emittance radio frequency electron guns and to obtain ultracold electrons for ultrafast electron diffraction applications.

Near atomically smooth alkali antimonide photocathode thin films

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

Feng, Jun; Karkare, Siddharth; Nasiatka, James

Nano-roughness is one of the major factors degrading the emittance of electron beams that can be generated by high efficiency photocathodes, such as the thermally reacted alkali antimonide thin films. In this paper, we demonstrate a co-deposition based method for producing alkali antimonide cathodes that produce near atomic smoothness with high reproducibility. Here, we calculate the effect of the surface roughness on the emittance and show that such smooth cathode surfaces are essential for operation of alkali antimonide cathodes in high field, low emittance radio frequency electron guns and to obtain ultracold electrons for ultrafast electron diffraction applications.

Ultrafast electron diffraction pattern simulations using GPU technology. Applications to lattice vibrations.

PubMed

Eggeman, A S; London, A; Midgley, P A

2013-11-01

Graphical processing units (GPUs) offer a cost-effective and powerful means to enhance the processing power of computers. Here we show how GPUs can greatly increase the speed of electron diffraction pattern simulations by the implementation of a novel method to generate the phase grating used in multislice calculations. The increase in speed is especially apparent when using large supercell arrays and we illustrate the benefits of fast encoding the transmission function representing the atomic potentials through the simulation of thermal diffuse scattering in silicon brought about by specific vibrational modes. © 2013 Elsevier B.V. All rights reserved.

Role of the Heat Sink Layer Ta for Ultrafast Spin Dynamic Process in Amorphous TbFeCo Thin Films

NASA Astrophysics Data System (ADS)

Ren, Y.; Zhang, Z. Z.; Min, T.; Jin, Q. Y.

The ultrafast demagnetization processes (UDP) in Ta (t nm)/TbFeCo (20 nm) films have been studied using the time-resolved magneto-optical Kerr effect (TRMOKE). With a fixed pump fluence of 2 mJ/cm2, for the sample without a Ta underlayer (t=0nm), we observed the UDP showing a two-step decay behavior, with a relatively longer decay time (τ2) around 3.0 ps in the second step due to the equilibrium of spin-lattice relaxation following the 4f occupation. As a 10nm Ta layer is deposited, the two-step demagnetization still exists while τ2 decreases to ˜1.9ps. Nevertheless, the second-step decay (τ2=0ps) disappears as the Ta layer thickness is increased up to 20 nm, only the first-step UDP occurs within 500 fs, followed by a fast recovery process. The rapid magnetization recovery rate strongly depends on the pump fluence. We infer that the Ta layer provides conduction electrons involving the thermal equilibrium of spin-lattice interaction and serves as heat bath taking away energy from spins of TbFeCo alloy film in UDP.

Obtaining Cross-Sections of Paint Layers in Cultural Artifacts Using Femtosecond Pulsed Lasers

PubMed Central

Harada, Takaaki; Spence, Stephanie; Margiolakis, Athanasios; Deckoff-Jones, Skylar; Ploeger, Rebecca; Shugar, Aaron N.; Hamm, James F.; Dani, Keshav M.; Dani, Anya R.

2017-01-01

Recently, ultrafast lasers exhibiting high peak powers and extremely short pulse durations have created a new paradigm in materials processing. The precision and minimal thermal damage provided by ultrafast lasers in the machining of metals and dielectrics also suggests a novel application in obtaining precise cross-sections of fragile, combustible paint layers in artwork and cultural heritage property. Cross-sections of paint and other decorative layers on artwork provide critical information into its history and authenticity. However, the current methodology which uses a scalpel to obtain a cross-section can cause further damage, including crumbling, delamination, and paint compression. Here, we demonstrate the ability to make controlled cross-sections of paint layers with a femtosecond pulsed laser, with minimal damage to the surrounding artwork. The femtosecond laser cutting overcomes challenges such as fragile paint disintegrating under scalpel pressure, or oxidation by the continuous-wave (CW) laser. Variations in laser power and translational speed of the laser while cutting exhibit different benefits for cross-section sampling. The use of femtosecond lasers in studying artwork also presents new possibilities in analyzing, sampling, and cleaning of artwork with minimal destructive effects. PMID:28772468

Temperature dependent of IVR investigated by steady-state and time-frequency resolved CARS for liquid nitrobenzene and nitromethane

NASA Astrophysics Data System (ADS)

Yang, Yanqiang; Zhu, Gangbei; Yan, Lin; Liu, Xiaosong; Yang's Ultrafast Spectroscopy Group Team

2017-06-01

Intramolecular vibrational energy redistribution (IVR) is important process in thermal decomposition, shock chemistry and photochemistry. Anti-Stokes Raman scattering is sensitive to the vibrational population in excited states because only vibrational excited states are responsible to the anti-Stokes Raman scattering, does not vibrational ground states. In this report, steady-state anti-Stokes Raman spectroscopy and broad band ultrafast coherent anti-Stokes Raman scattering (CARS) are performed. The steady-state anti-Stokes Raman spectroscopy shows temperature dependent of vibrational energy redistribution in vibrational excited-state molecule, and reveal that, in liquid nitrobenzene, with temperature increasing, vibrational energy is mainly redistributed in NO2 symmetric stretching mode, and phenyl ring stretching mode of νCC. For liquid nitromethane, it is found that, with temperature increasing, vibrational energy concentrate in CN stretching mode and methyl umbrella vibrational mode. In the broad band ultrafast CARS experiment, multiple vibrational modes are coherently excited to vibrational excited states, and the time-frequency resolved CARS spectra show the coincident IVR processes. This work is supported by the National Natural Science Foundation of China (Grant Numbers 21673211 and 11372053), and the Science Challenging Program (Grant Number JCKY2016212A501).

Effect of Ultra-Fast Cooling on Microstructure and Properties of High Strength Steel for Shipbuilding

NASA Astrophysics Data System (ADS)

Zhou, Cheng; Ye, Qibin; Yan, Ling

The effect of ultra-fast cooling(UFC) and conventional accelerated cooling(AcC) on the mechanical properties and microstructure of controlled rolled AH32 grade steel plates on industrial scale were compared using tensile test, Charpy impact test, welding thermal simulation, and microscopic analysis. The results show that the properties of the plate produced by UFC are improved considerably comparing to that by AcC. The yield strength is increased with 54 MPa without deterioration in the ductility and the impact energy is improved to more than 260 J at -60 °C with much lower ductile-to-brittle transition temperature(DBTT). The ferrite grain size is refined to ASTM No. 11.5 in the UFC steel with uniform microstructure throughout the thickness direction, while that of the AcC steel is ASTM No. 9.5. The analysis of nucleation kinetics of α-ferrite indicates that the microstructure is refined due to the increased nucleation rate of α-ferrite by much lower γ→α transition temperature through the UFC process. The Hall-Petch effect is quantified for the improvement of the strength and toughness of the UFC steel attributed to the grain refinement.

Trends in laser micromachining

NASA Astrophysics Data System (ADS)

Gaebler, Frank; van Nunen, Joris; Held, Andrew

2016-03-01

Laser Micromachining is well established in industry. Depending on the application lasers with pulse length from μseconds to femtoseconds and wavelengths from 1064nm and its harmonics up to 5μm or 10.6μm are used. Ultrafast laser machining using pulses with pico or femtosecond duration pulses is gaining traction, as it offers very precise processing of materials with low thermal impact. Large-scale industrial ultrafast laser applications show that the market can be divided into various sub segments. One set of applications demand low power around 10W, compact footprint and are extremely sensitive to the laser price whilst still demanding 10ps or shorter laser pulses. A second set of applications are very power hungry and only become economically feasible for large scale deployments at power levels in the 100+W class. There is also a growing demand for applications requiring fs-laser pulses. In our presentation we would like to describe these sub segments by using selected applications from the automotive and electronics industry e.g. drilling of gas/diesel injection nozzles, dicing of LED substrates. We close the presentation with an outlook to micromachining applications e.g. glass cutting and foil processing with unique new CO lasers emitting 5μm laser wavelength.

Obtaining Cross-Sections of Paint Layers in Cultural Artifacts Using Femtosecond Pulsed Lasers.

PubMed

Harada, Takaaki; Spence, Stephanie; Margiolakis, Athanasios; Deckoff-Jones, Skylar; Ploeger, Rebecca; Shugar, Aaron N; Hamm, James F; Dani, Keshav M; Dani, Anya R

2017-01-26

Recently, ultrafast lasers exhibiting high peak powers and extremely short pulse durations have created a new paradigm in materials processing. The precision and minimal thermal damage provided by ultrafast lasers in the machining of metals and dielectrics also suggests a novel application in obtaining precise cross-sections of fragile, combustible paint layers in artwork and cultural heritage property. Cross-sections of paint and other decorative layers on artwork provide critical information into its history and authenticity. However, the current methodology which uses a scalpel to obtain a cross-section can cause further damage, including crumbling, delamination, and paint compression. Here, we demonstrate the ability to make controlled cross-sections of paint layers with a femtosecond pulsed laser, with minimal damage to the surrounding artwork. The femtosecond laser cutting overcomes challenges such as fragile paint disintegrating under scalpel pressure, or oxidation by the continuous-wave (CW) laser. Variations in laser power and translational speed of the laser while cutting exhibit different benefits for cross-section sampling. The use of femtosecond lasers in studying artwork also presents new possibilities in analyzing, sampling, and cleaning of artwork with minimal destructive effects.

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.

Ultrafast Science Opportunities with Electron Microscopy

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

Durr, Hermann

X-rays and electrons are two of the most fundamental probes of matter. When the Linac Coherent Light Source (LCLS), the world’s first x-ray free electron laser, began operation in 2009, it transformed ultrafast science with the ability to generate laser-like x-ray pulses from the manipulation of relativistic electron beams. This document describes a similar future transformation. In Transmission Electron Microscopy, ultrafast relativistic (MeV energy) electron pulses can achieve unsurpassed spatial and temporal resolution. Ultrafast temporal resolution will be the next frontier in electron microscopy and can ideally complement ultrafast x-ray science done with free electron lasers. This document describes themore » Grand Challenge science opportunities in chemistry, material science, physics and biology that arise from an MeV ultrafast electron diffraction & microscopy facility, especially when coupled with linac-based intense THz and X-ray pump capabilities.« less

Self-phase modulation enabled, wavelength-tunable ultrafast fiber laser sources: an energy scalable approach.

PubMed

Liu, Wei; Li, Chen; Zhang, Zhigang; Kärtner, Franz X; Chang, Guoqing

2016-07-11

We propose and demonstrate a new approach to implement a wavelength-tunable ultrafast fiber laser source suitable for multiphoton microscopy. We employ fiber-optic nonlinearities to broaden a narrowband optical spectrum generated by an Yb-fiber laser system and then use optical bandpass filters to select the leftmost or rightmost spectral lobes from the broadened spectrum. Detailed numerical modeling shows that self-phase modulation dominates the spectral broadening, self-steepening tends to blue shift the broadened spectrum, and stimulated Raman scattering is minimal. We also find that optical wave breaking caused by fiber dispersion slows down the shift of the leftmost/rightmost spectral lobes and therefore limits the wavelength tuning range of the filtered spectra. We show both numerically and experimentally that shortening the fiber used for spectral broadening while increasing the input pulse energy can overcome this dispersion-induced limitation; as a result, the filtered spectral lobes have higher power, constituting a powerful and practical approach for energy scaling the resulting femtosecond sources. We use two commercially available photonic crystal fibers to verify the simulation results. More specific, use of 20-mm fiber NL-1050-ZERO-2 enables us to implement an Yb-fiber laser based ultrafast source, delivering femtosecond (70-120 fs) pulses tunable from 825 nm to 1210 nm with >1 nJ pulse energy.

Multi-phase functionalization of titanium for enhanced photon absorption in the vis-NIR region.

PubMed

Thakur, Pooja; Tan, Bo; Venkatakrishnan, Krishnan

2015-10-19

Inadequate absorption of Near Infrared (NIR) photons by conventional silicon solar cells has been a major stumbling block towards the attainment of a high efficiency "full spectrum" solar cell. An effective enhancement in the absorption of such photons is desired as they account for a considerable portion of the tappable solar energy. In this work, we report a remarkable gain observed in the absorption of photons in the near infrared and visible region (400 nm-1000 nm) by a novel multi-phased oxide of titanium. Synthesised via a single step ultra-fast laser pulse interaction with pure titanium, characterisation studies have identified this oxide of titanium to be multi-phased and composed of Ti3O, (TiO.716)3.76 and TiO2 (rutile). Computed to have an average band gap value of 2.39 eV, this ultrafast laser induced multi-phased titanium oxide has especially exhibited steady absorption capability in the NIR range of 750-1000 nm, which to the best of our knowledge, was never reported before. The unique NIR absorption properties of the laser functionalised titanium coupled with the simplicity and versatility of the ultrafast laser interaction process involved thereby provides tremendous potential towards the photon sensitization of titanium and thereafter for the inception of a "full spectrum" solar device.

Infrared laser damage thresholds in corneal tissue phantoms using femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Boretsky, Adam R.; Clary, Joseph E.; Noojin, Gary D.; Rockwell, Benjamin A.

2018-02-01

Ultrafast lasers have become a fixture in many biomedical, industrial, telecommunications, and defense applications in recent years. These sources are capable of generating extremely high peak power that can cause laser-induced tissue breakdown through the formation of a plasma upon exposure. Despite the increasing prevalence of such lasers, current safety standards (ANSI Z136.1-2014) do not include maximum permissible exposure (MPE) values for the cornea with pulse durations less than one nanosecond. This study was designed to measure damage thresholds in corneal tissue phantoms in the near-infrared and mid-infrared to identify the wavelength dependence of laser damage thresholds from 1200-2500 nm. A high-energy regenerative amplifier and optical parametric amplifier outputting 100 femtosecond pulses with pulse energies up to 2 mJ were used to perform exposures and determine damage thresholds in transparent collagen gel tissue phantoms. Three-dimensional imaging, primarily optical coherence tomography, was used to evaluate tissue phantoms following exposure to determine ablation characteristics at the surface and within the bulk material. The determination of laser damage thresholds in the near-IR and mid-IR for ultrafast lasers will help to guide safety standards and establish the appropriate MPE levels for exposure sensitive ocular tissue such as the cornea. These data will help promote the safe use of ultrafast lasers for a wide range of applications.

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.

Characterization of fast photoelectron packets in weak and strong laser fields in ultrafast electron microscopy.

PubMed

Plemmons, Dayne A; Tae Park, Sang; Zewail, Ahmed H; Flannigan, David J

2014-11-01

The development of ultrafast electron microscopy (UEM) and variants thereof (e.g., photon-induced near-field electron microscopy, PINEM) has made it possible to image atomic-scale dynamics on the femtosecond timescale. Accessing the femtosecond regime with UEM currently relies on the generation of photoelectrons with an ultrafast laser pulse and operation in a stroboscopic pump-probe fashion. With this approach, temporal resolution is limited mainly by the durations of the pump laser pulse and probe electron packet. The ability to accurately determine the duration of the electron packets, and thus the instrument response function, is critically important for interpretation of dynamics occurring near the temporal resolution limit, in addition to quantifying the effects of the imaging mode. Here, we describe a technique for in situ characterization of ultrashort electron packets that makes use of coupling with photons in the evanescent near-field of the specimen. We show that within the weakly-interacting (i.e., low laser fluence) regime, the zero-loss peak temporal cross-section is precisely the convolution of electron packet and photon pulse profiles. Beyond this regime, we outline the effects of non-linear processes and show that temporal cross-sections of high-order peaks explicitly reveal the electron packet profile, while use of the zero-loss peak becomes increasingly unreliable. Copyright © 2014 Elsevier B.V. All rights reserved.

Measuring phonon mean free path distributions by probing quasiballistic phonon transport in grating nanostructures

DOE PAGES

Zeng, Lingping; Collins, Kimberlee C.; Hu, Yongjie; ...

2015-11-27

Heat conduction in semiconductors and dielectrics depends upon their phonon mean free paths that describe the average travelling distance between two consecutive phonon scattering events. Nondiffusive phonon transport is being exploited to extract phonon mean free path distributions. Here, we describe an implementation of a nanoscale thermal conductivity spectroscopy technique that allows for the study of mean free path distributions in optically absorbing materials with relatively simple fabrication and a straightforward analysis scheme. We pattern 1D metallic grating of various line widths but fixed gap size on sample surfaces. The metal lines serve as both heaters and thermometers in time-domainmore » thermoreflectance measurements and simultaneously act as wiregrid polarizers that protect the underlying substrate from direct optical excitation and heating. We demonstrate the viability of this technique by studying length-dependent thermal conductivities of silicon at various temperatures. The thermal conductivities measured with different metal line widths are analyzed using suppression functions calculated from the Boltzmann transport equation to extract the phonon mean free path distributions with no calibration required. Furthermore, this table-top ultrafast thermal transport spectroscopy technique enables the study of mean free path spectra in a wide range of technologically important materials.« less

Kinetic Monte Carlo simulations for transient thermal fields: Computational methodology and application to the submicrosecond laser processes in implanted silicon.

PubMed

Fisicaro, G; Pelaz, L; Lopez, P; La Magna, A

2012-09-01

Pulsed laser irradiation of damaged solids promotes ultrafast nonequilibrium kinetics, on the submicrosecond scale, leading to microscopic modifications of the material state. Reliable theoretical predictions of this evolution can be achieved only by simulating particle interactions in the presence of large and transient gradients of the thermal field. We propose a kinetic Monte Carlo (KMC) method for the simulation of damaged systems in the extremely far-from-equilibrium conditions caused by the laser irradiation. The reference systems are nonideal crystals containing point defect excesses, an order of magnitude larger than the equilibrium density, due to a preirradiation ion implantation process. The thermal and, eventual, melting problem is solved within the phase-field methodology, and the numerical solutions for the space- and time-dependent thermal field were then dynamically coupled to the KMC code. The formalism, implementation, and related tests of our computational code are discussed in detail. As an application example we analyze the evolution of the defect system caused by P ion implantation in Si under nanosecond pulsed irradiation. The simulation results suggest a significant annihilation of the implantation damage which can be well controlled by the laser fluence.

Physical mechanisms of SiN{sub x} layer structuring with ultrafast lasers by direct and confined laser ablation

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

Rapp, S., E-mail: rapp@hm.edu; Erlangen Graduate School in Advanced Optical Technologies; Heinrich, G.

2015-03-14

In the production process of silicon microelectronic devices and high efficiency silicon solar cells, local contact openings in thin dielectric layers are required. Instead of photolithography, these openings can be selectively structured with ultra-short laser pulses by confined laser ablation in a fast and efficient lift off production step. Thereby, the ultrafast laser pulse is transmitted by the dielectric layer and absorbed at the substrate surface leading to a selective layer removal in the nanosecond time domain. Thermal damage in the substrate due to absorption is an unwanted side effect. The aim of this work is to obtain a deepermore » understanding of the physical laser-material interaction with the goal of finding a damage-free ablation mechanism. For this, thin silicon nitride (SiN{sub x}) layers on planar silicon (Si) wafers are processed with infrared fs-laser pulses. Two ablation types can be distinguished: The known confined ablation at fluences below 300 mJ/cm{sup 2} and a combined partial confined and partial direct ablation at higher fluences. The partial direct ablation process is caused by nonlinear absorption in the SiN{sub x} layer in the center of the applied Gaussian shaped laser pulses. Pump-probe investigations of the central area show ultra-fast reflectivity changes typical for direct laser ablation. Transmission electron microscopy results demonstrate that the Si surface under the remaining SiN{sub x} island is not damaged by the laser ablation process. At optimized process parameters, the method of direct laser ablation could be a good candidate for damage-free selective structuring of dielectric layers on absorbing substrates.« less

PREFACE: Ultrafast and nonlinear optics in carbon nanomaterials

NASA Astrophysics Data System (ADS)

Kono, Junichiro

2013-02-01

Carbon-based nanomaterials—single-wall carbon nanotubes (SWCNTs) and graphene, in particular—have emerged in the last decade as novel low-dimensional systems with extraordinary properties. Because they are direct-bandgap systems, SWCNTs are one of the leading candidates to unify electronic and optical functions in nanoscale circuitry; their diameter-dependent bandgaps can be utilized for multi-wavelength devices. Graphene's ultrahigh carrier mobilities are promising for high-frequency electronic devices, while, at the same time, it is predicted to have ideal properties for terahertz generation and detection due to its unique zero-gap, zero-mass band structure. There have been a large number of basic optical studies on these materials, but most of them were performed in the weak-excitation, quasi-equilibrium regime. In order to probe and assess their performance characteristics as optoelectronic materials under device-operating conditions, it is crucial to strongly drive them and examine their optical properties in highly non-equilibrium situations and with ultrashot time resolution. In this section, the reader will find the latest results in this rapidly growing field of research. We have assembled contributions from some of the leading experts in ultrafast and nonlinear optical spectroscopy of carbon-based nanomaterials. Specific topics featured include: thermalization, cooling, and recombination dynamics of photo-generated carriers; stimulated emission, gain, and amplification; ultrafast photoluminescence; coherent phonon dynamics; exciton-phonon and exciton-plasmon interactions; exciton-exciton annihilation and Auger processes; spontaneous and stimulated emission of terahertz radiation; four-wave mixing and harmonic generation; ultrafast photocurrents; the AC Stark and Franz-Keldysh effects; and non-perturbative light-mater coupling. We would like to express our sincere thanks to those who contributed their latest results to this special section, and the Journal of Physics: Condensed Matter staff for their help, patience and professionalism. Since this is a fast-moving field, there is absolutely no way of presenting definitive answers to all open questions, but we hope that this special section will provide an overview of the current state of knowledge regarding this topic. Furthermore, we hope that the exciting science and technology described in this section will attract and inspire other researchers and students working in related fields to enter into the study of ultrafast and nonlinear optical phenomena in carbon-based nanostructures. Ultrafast and nonlinear optics in carbon nanomaterials contents Ultrafast and nonlinear optics in carbon nanomaterialsJunichiro Kono The impact of pump fluence on carrier relaxation dynamics in optically excited grapheneT Winzer and E Malic Time-resolved spectroscopy on epitaxial graphene in the infrared spectral range: relaxation dynamics and saturation behaviorS Winnerl, F Göttfert, M Mittendorff, H Schneider, M Helm, T Winzer, E Malic, A Knorr, M Orlita, M Potemski, M Sprinkle, C Berger and W A de Heer Nonlinear optics of graphene in a strong magnetic fieldXianghan Yao and Alexey Belyanin Theory of coherent phonons in carbon nanotubes and graphene nanoribbonsG D Sanders, A R T Nugraha, K Sato, J-H Kim3, J Kono3, R Saito and C J Stanton Non-perturbative effects of laser illumination on the electrical properties of graphene nanoribbons Hernán L Calvo, Pablo M Perez-Piskunow, Horacio M Pastawski, Stephan Roche and Luis E F Foa Torres Transient absorption microscopy studies of energy relaxation in graphene oxide thin film Sean Murphy and Libai Huang Femtosecond dynamics of exciton localization: self-trapping from the small to the large polaron limit F X Morrissey, J G Mance, A D Van Pelt and S L Dexheimer

Modeling of Ultrafast Laser Induced Electron Emission from TI and Graphene

DTIC Science & Technology

2017-09-08

and Design Final Report 09/08/2017 DISTRIBUTION A: Distribution approved for public release. AF Office Of Scientific Research (AFOSR)/ IOA Arlington... Design 287 GHIM MOH ROAD Singapore, 279623 SG 8. PERFORMING ORGANIZATION REPORT NUMBER 9. SPONSORING/MONITORING AGENCY NAME(S) AND ADDRESS(ES) AOARD...of Technology and Design - Mailing Address : 8 Somapah Road, Singapore 487372 - Phone : (65) 6499 4558 - Fax : NIL Period of Performance: 16

Numerical Simulation of Ultra-Fast Pulse Propagation in Two-Photon Absorbing Medium

DTIC Science & Technology

2011-08-01

physical problems including coherent- and incoherent regimes of optical power limiting, saturation, CEP effects, soliton formation etc. It can be also...coherent- and incoherent regimes of optical power limiting, saturation, CEP effects, electromagnetically induced transparency, soliton formation etc...experimental data ( dark blue); Upper panel - 1PA spectrum; Lower panel - 2PA cross section spectrum. The parameter values used are shown in Table 1. 10

Frequency-tunable continuous-wave terahertz sources based on GaAs plasmonic photomixers

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

Yang, Shang-Hua; Jarrahi, Mona; Electrical Engineering Department, University of California Los Angeles, Los Angeles, California 90095

2015-09-28

We present frequency-tunable, continuous-wave terahertz sources based on GaAs plasmonic photomixers, which offer high terahertz radiation power levels at 50% radiation duty cycle. The use of plasmonic contact electrodes enhances photomixer quantum efficiency while maintaining its ultrafast operation by concentrating a large number of photocarriers in close proximity to the device contact electrodes. Additionally, the relatively high thermal conductivity and high resistivity of GaAs allow operation under high optical pump power levels and long duty cycles without reaching the thermal breakdown limit of the photomixer. We experimentally demonstrate continuous-wave terahertz radiation with a radiation frequency tuning range of more thanmore » 2 THz and a record-high radiation power of 17 μW at 1 THz through plasmonic photomixers fabricated on a low temperature grown GaAs substrate at 50% radiation duty cycle.« less

Electronic cooling via interlayer Coulomb coupling in multilayer epitaxial graphene

PubMed Central

Mihnev, Momchil T.; Tolsma, John R.; Divin, Charles J.; Sun, Dong; Asgari, Reza; Polini, Marco; Berger, Claire; de Heer, Walt A.; MacDonald, Allan H.; Norris, Theodore B.

2015-01-01

In van der Waals bonded or rotationally disordered multilayer stacks of two-dimensional (2D) materials, the electronic states remain tightly confined within individual 2D layers. As a result, electron–phonon interactions occur primarily within layers and interlayer electrical conductivities are low. In addition, strong covalent in-plane intralayer bonding combined with weak van der Waals interlayer bonding results in weak phonon-mediated thermal coupling between the layers. We demonstrate here, however, that Coulomb interactions between electrons in different layers of multilayer epitaxial graphene provide an important mechanism for interlayer thermal transport, even though all electronic states are strongly confined within individual 2D layers. This effect is manifested in the relaxation dynamics of hot carriers in ultrafast time-resolved terahertz spectroscopy. We develop a theory of interlayer Coulomb coupling containing no free parameters that accounts for the experimentally observed trends in hot-carrier dynamics as temperature and the number of layers is varied. PMID:26399955

Laser-induced damage threshold tests of ultrafast multilayer dielectric coatings in various environmental conditions relevant for operation of ELI beamlines laser systems

NASA Astrophysics Data System (ADS)

Ďurák, Michal; Velpula, Praveen Kumar; Kramer, Daniel; Cupal, Josef; Medřík, Tomáš; Hřebíček, Jan; Golasowski, Jiří; Peceli, Davorin; Kozlová, Michaela; Rus, Bedřich

2017-01-01

Increasing the laser-induced damage resistance of optical components is one of the major challenges in the development of Peta-watt (PW) class laser systems. The extreme light infrastructure (ELI) beamlines project will provide ultrafast laser systems with peak powers up to 10 PW available every minute and PW class beams at 10 Hz complemented by a 5-TW, 1-kHz beamline. Sustainable performance of PW class laser systems relies on the durability of the employed optical components. As part of an effort to evaluate the damage resistance of components utilized in ELI beamlines systems, damage thresholds of several optical multilayer dielectric coatings were measured with different laser parameters and in different environments. Three coatings were tested with 10 Hz and 1 kHz pulse repetition rates, and the effect of a cleaning treatment on their damage resistance was examined. To explore the damage threshold behavior at different vacuum levels, one coating was subject to tests at various residual gas pressures. No change of damage threshold in a high vacuum with respect to ambient pressure was recorded. The effect of the cleaning treatment was found to be inconsistent, suggesting that development of the optimal cleaning treatment for a given coating requires consideration of its specific properties.

Optical and Nonlinear Optical Response of Light Sensor Thin Films

PubMed Central

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

2005-01-01

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

High-frequency polarization dynamics in spin-lasers: pushing the limits

NASA Astrophysics Data System (ADS)

Gerhardt, Nils C.; Lindemann, Markus; Pusch, Tobias; Michalzik, Rainer; Hofmann, Martin R.

2017-09-01

While the high-frequency performance of conventional lasers is limited by the coupled carrier-photon dynamics, spin-polarized lasers have a high potential to overcome this limitation and to push the direct modulation bandwidth beyond 100 GHz. The key is to utilize the ultrafast polarization dynamics in spin-polarized vertical cavity surface-emitting lasers (spin-VCSELs) which is decoupled from the intensity dynamics and its fundamental limitations. The polarization dynamics in such devices, characterized by the polarization oscillation resonance frequency, is mainly determined by the amount of birefringence in the cavity. Using an approach for manipulating the birefringence via mechanical strain we were able to increase the polarization dynamics to resonance frequencies of more than 40 GHz. Up to now these values are only limited by the setup to induce birefringence and do not reflect any fundamental limitations. Taking our record results for the birefringence-induced mode splitting of more than 250 GHz into account, the concept has the potential to provide polarization modulation in spin-VCSELs with modulation frequencies far beyond 100 GHz. This makes them ideal devices for next-generation fast optical interconnects. In this paper we present experimental results for ultrafast polarization dynamics up to 50 GHz and compare them to numerical simulations.

Imaging ultrafast dynamics of molecules with laser-induced electron diffraction.

PubMed

Lin, C D; Xu, Junliang

2012-10-14

We introduce a laser-induced electron diffraction method (LIED) for imaging ultrafast dynamics of small molecules with femtosecond mid-infrared lasers. When molecules are placed in an intense laser field, both low- and high-energy photoelectrons are generated. According to quantitative rescattering (QRS) theory, high-energy electrons are produced by a rescattering process where electrons born at the early phase of the laser pulse are driven back to rescatter with the parent ion. From the high-energy electron momentum spectra, field-free elastic electron-ion scattering differential cross sections (DCS), or diffraction images, can be extracted. With mid-infrared lasers as the driving pulses, it is further shown that the DCS can be used to extract atomic positions in a molecule with sub-angstrom spatial resolution, in close analogy to the standard electron diffraction method. Since infrared lasers with pulse duration of a few to several tens of femtoseconds are already available, LIED can be used for imaging dynamics of molecules with sub-angstrom spatial and a few-femtosecond temporal resolution. The first experiment with LIED has shown that the bond length of oxygen molecules shortens by 0.1 Å in five femtoseconds after single ionization. The principle behind LIED and its future outlook as a tool for dynamic imaging of molecules are presented.

Hydration-reduced lattice thermal conductivity of olivine in Earth’s upper mantle

PubMed Central

Chang, Yun-Yuan; Hsieh, Wen-Pin; Tan, Eh; Chen, Jiuhua

2017-01-01

Earth’s water cycle enables the incorporation of water (hydration) in mantle minerals that can influence the physical properties of the mantle. Lattice thermal conductivity of mantle minerals is critical for controlling the temperature profile and dynamics of the mantle and subducting slabs. However, the effect of hydration on lattice thermal conductivity remains poorly understood and has often been assumed to be negligible. Here we have precisely measured the lattice thermal conductivity of hydrous San Carlos olivine (Mg0.9Fe0.1)2SiO4 (Fo90) up to 15 gigapascals using an ultrafast optical pump−probe technique. The thermal conductivity of hydrous Fo90 with ∼7,000 wt ppm water is significantly suppressed at pressures above ∼5 gigapascals, and is approximately 2 times smaller than the nominally anhydrous Fo90 at mantle transition zone pressures, demonstrating the critical influence of hydration on the lattice thermal conductivity of olivine in this region. Modeling the thermal structure of a subducting slab with our results shows that the hydration-reduced thermal conductivity in hydrated oceanic crust further decreases the temperature at the cold, dry center of the subducting slab. Therefore, the olivine−wadsleyite transformation rate in the slab with hydrated oceanic crust is much slower than that with dry oceanic crust after the slab sinks into the transition zone, extending the metastable olivine to a greater depth. The hydration-reduced thermal conductivity could enable hydrous minerals to survive in deeper mantle and enhance water transportation to the transition zone. PMID:28377520

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.

Laser-induced THz magnetization precession for a tetragonal Heusler-like nearly compensated ferrimagnet

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

Mizukami, S., E-mail: mizukami@wpi-aimr.tohoku.ac.jp; Sugihara, A.; Suzuki, K. Z.

2016-01-04

Laser-induced magnetization precessional dynamics was investigated in epitaxial films of Mn{sub 3}Ge, which is a tetragonal Heusler-like nearly compensated ferrimagnet. The ferromagnetic resonance (FMR) mode was observed, the precession frequency for which exceeded 0.5 THz and originated from the large magnetic anisotropy field of approximately 200 kOe for this ferrimagnet. The effective damping constant was approximately 0.03. The corresponding effective Landau-Lifshitz constant is approximately 60 Mrad/s and is comparable with those of the similar Mn-Ga materials. The physical mechanisms for the Gilbert damping and for the laser-induced excitation of the FMR mode were also discussed in terms of the spin-orbit-induced damping and themore » laser-induced ultrafast modulation of the magnetic anisotropy, respectively.« less

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

FOREWORD: The 12th International Workshop on Desorption Induced by Electronic Transitions (DIET XII) (Pine Mountain, Georgia, USA, 19-23 April 2009) The 12th International Workshop on Desorption Induced by Electronic Transitions (DIET XII) (Pine Mountain, Georgia, USA, 19-23 April 2009)

NASA Astrophysics Data System (ADS)

Orlando, Thomas M.; Diebold, Ulrike

2010-03-01

The 12th International Workshop on Desorption Induced by Electronic Transitions (DIET XII) took place from 19-23 April 2009 in Pine Mountain, Georgia, USA. This was the 12th conference in a strong and vibrant series, which dates back to the early 1980s. DIET XII continued the tradition of exceptional interdisciplinary science and focused on the study of desorption and dynamics induced by electronic excitations of surfaces and interfaces. The format involved invited lectures, contributed talks and a poster session on the most recent developments and advances in this area of surface physics. The Workshop International Steering Committee and attendees wish to dedicate DIET XII to the memory of the late Professor Theodore (Ted) Madey. Ted was one of the main pioneers of this field and was one of the primary individuals working to keep this area of science exciting and adventurous. His overall contributions to surface science were countless and his contributions to the DIET field and community were enormous. He is missed and remembered by many friends and colleagues throughout the world. The papers collected in this issue cover many of the highlights of DIET XII. Topics include ultrafast electron transfer at surfaces and interfaces, quantum and spatially resolved mapping of surface dynamics and desorption, photon-, electron- and ion-beam induced processes at complex interfaces, the role of non-thermal desorption in astrochemistry and astrophysics and laser-/ion-based methods of examining soft matter and biological media. Although the workshop attracted many scientists active in the general area of non-thermal surface processes, DIET XII also attracted many younger scientists (i.e., postdoctoral fellows, advanced graduate students, and a select number of advanced undergraduate students). This field has had an impact in a number of areas including nanoscience, device physics, astrophysics, and now biophysics. We believe that this special issue of Journal of Physics: Condensed Matter will help foster further progress in the study of DIET processes. Since the field remains vibrant and exciting, the workshop series will continue with DIET XIII. Professor Richard Palmer (University of Birmingham, UK) will chair DIET XIII in the UK in early summer 2012. We gratefully acknowledge financial support from SPECS, HIDEN Analytical, BRUKER, The United States National Science Foundation, Georgia Institute of Technology and The State University of New Jersey, Rutgers.

Study on Ultrafast Photodynamics of Novel Multilayered Thin Films for Device Applications

DTIC Science & Technology

2004-07-31

study ultrafast phase-transition of VO2 thin film. This part of work was started right after the new laser installed. With better laser output...1-3]. With the purpose of combined effect that the proposed ultrafast phase-transition VO2 thin film deposited on a substrate of heavy metal...second point of focus was to study ultrafast phase-transition of VO2 thin film. This part of work was started right after the new laser installed

Direct-write maskless lithography using patterned oxidation of Si-substrate Induced by femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Kiani, Amirkianoosh; Venkatakrishnan, Krishnan; Tan, Bo

2013-03-01

In this study we report a new method for direct-write maskless lithography using oxidized silicon layer induced by high repetition (MHz) ultrafast (femtosecond) laser pulses under ambient condition. The induced thin layer of predetermined pattern can act as an etch stop during etching process in alkaline etchants such as KOH. The proposed method can be leading to promising solutions for direct-write maskless lithography technique since the proposed method offers a higher degree of flexibility and reduced time and cost of fabrication which makes it particularly appropriate for rapid prototyping and custom scale manufacturing. A Scanning Electron Microscope (SEM), Micro-Raman, Energy Dispersive X-ray (EDX), optical microscope and X-ray diffraction spectroscopy (XRD) were used to evaluate the quality of oxidized layer induced by laser pulses.

Laser-induced spin protection and switching in a specially designed magnetic dot: A theoretical investigation

NASA Astrophysics Data System (ADS)

Zhang, G. P.; Si, M. S.; George, T. F.

2011-04-01

Most laser-induced femtosecond magnetism investigations are done in magnetic thin films. Nanostructured magnetic dots, with their reduced dimensionality, present new opportunities for spin manipulation. Here we predict that if a magnetic dot has a dipole-forbidden transition between the lowest occupied molecular orbital (LUMO) and the highest unoccupied molecular orbital (HOMO), but a dipole-allowed transition between LUMO+1 and HOMO, electromagnetically induced transparency can be used to prevent ultrafast laser-induced spin momentum reduction, or spin protection. This is realized through a strong dump pulse to funnel the population into LUMO+1. If the time delay between the pump and dump pulses is longer than 60 fs, a population inversion starts and spin switching is achieved. These predictions are detectable experimentally.

Direct anisotropic growth of CdS nanocrystals in thermotropic liquid crystal templates for heterojunction optoelectronics.

PubMed

Yuan, Kai; Chen, Lie; Chen, Yiwang

2014-09-01

The direct growth of CdS nanocrystals in functional solid-state thermotropic liquid crystal (LC) small molecules and a conjugated LC polymer by in situ thermal decomposition of a single-source cadmium xanthate precursor to fabricate LC/CdS hybrid nanocomposites is described. The influence of thermal annealing temperature of the LC/CdS precursors upon the nanomorphology, photophysics, and optoelectronic properties of the LC/CdS nanocomposites is systematically studied. Steady-state PL and ultrafast emission dynamics studies show that the charge-transfer rates are strongly dependent on the thermal annealing temperature. Notably, annealing at liquid-crystal state temperature promotes a more organized nanomorphology of the LC/CdS nanocomposites with improved photophysics and optoelectronic properties. The results confirm that thermotropic LCs can be ideal candidates as organization templates for the control of organic/inorganic hybrid nanocomposites at the nanoscale level. The results also demonstrate that in situ growth of semiconducting nanocrystals in thermotropic LCs is a versatile route to hybrid organic/inorganic nanocomposites and optoelectronic devices. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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.

Structure-dependent water transport across nanopores of carbon nanotubes: toward selective gating upon temperature regulation.

PubMed

Zhao, Kuiwen; Wu, Huiying

2015-04-28

Determining water structure in nanopores and its influence on water transport behaviour is of great importance for understanding and regulating the transport across nanopores. Here we report an ultrafast-slow flow transition phenomenon for water transport across nanopores of carbon nanotubes owing to the change in water structure in nanopores induced by temperature. By performing extensive molecular dynamics simulations, we show the dependence of water transport behaviours on water structures. Our results indicate that owing to the change in water structure in nanopores, water flux across nanopores with certain pore sizes decreases sharply (nearly 3 orders of magnitude) with the decreasing temperature. This phenomenon is very sensitive to the pore size. The threshold temperatures for the occurrence of the ultrafast-slow flow transition for water transport are also determined for various pore sizes. These findings suggest a novel protocol for selective gating of water and proton conduction across nanopores and temperature-controlled drug release.

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

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

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

Correlated terahertz acoustic and electromagnetic emission in dynamically screened InGaN/GaN quantum wells

NASA Astrophysics Data System (ADS)

van Capel, P. J. S.; Turchinovich, D.; Porte, H. P.; Lahmann, S.; Rossow, U.; Hangleiter, A.; Dijkhuis, J. I.

2011-08-01

We investigate acoustic and electromagnetic emission from optically excited strained piezoelectric In0.2Ga0.8N/GaN multiple quantum wells (MQWs), using optical pump-probe spectroscopy, time-resolved Brillouin scattering, and THz emission spectroscopy. A direct comparison of detected acoustic signals and THz electromagnetic radiation signals demonstrates that transient strain generation in InGaN/GaN MQWs is correlated with electromagnetic THz generation, and both types of emission find their origin in ultrafast dynamical screening of the built-in piezoelectric field in the MQWs. The measured spectral intensity of the detected Brillouin signal corresponds to a maximum strain amplitude of generated acoustic pulses of 2%. This value coincides with the static lattice-mismatch-induced strain in In0.2Ga0.8N/GaN, demonstrating the total release of static strain in MQWs via impulsive THz acoustic emission. This confirms the ultrafast dynamical screening mechanism in MQWs as a highly efficient method for impulsive strain generation.

Stacking order dynamics in the quasi-two-dimensional dichalcogenide 1 T-TaS 2 probed with MeV ultrafast electron diffraction

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

Le Guyader, L.; Chase, T.; Reid, A. H.

Transitions between different charge density wave (CDW) states in quasi-two-dimensional materials may be accompanied also by changes in the inter-layer stacking of the CDW. Using MeV ultrafast electron diffraction, the out-of-plane stacking order dynamics in the quasi-two-dimensional dichalcogenide 1 T-TaS 2 is investigated for the first time. From the intensity of the CDW satellites aligned around the commensurate l = 1/6 characteristic stacking order, it is found out that this phase disappears with a 0.3 ps time constant. Simultaneously, in the same experiment, the emergence of the incommensurate phase, with a slightly slower 2.0 ps time constant, is determined frommore » the intensity of the CDW satellites aligned around the incommensurate l = 1/3 characteristic stacking order. Finally, these results might be of relevance in understanding the metallic character of the laser-induced metastable “hidden” state recently discovered in this compound.« less

Dynamic x-ray imaging of laser-driven nanoplasmas

NASA Astrophysics Data System (ADS)

Fennel, Thomas

2016-05-01

A major promise of current x-ray science at free electron lasers is the realization of unprecedented imaging capabilities for resolving the structure and ultrafast dynamics of matter with nanometer spatial and femtosecond temporal resolution or even below via single-shot x-ray diffraction. Laser-driven atomic clusters and nanoparticles provide an ideal platform for developing and demonstrating the required technology to extract the ultrafast transient spatiotemporal dynamics from the diffraction images. In this talk, the perspectives and challenges of dynamic x-ray imaging will be discussed using complete self-consistent microscopic electromagnetic simulations of IR pump x-ray probe imaging for the example of clusters. The results of the microscopic particle-in-cell simulations (MicPIC) enable the simulation-assisted reconstruction of corresponding experimental data. This capability is demonstrated by converting recently measured LCLS data into a ultrahigh resolution movie of laser-induced plasma expansion. Finally, routes towards reaching attosecond time resolution in the visualization of complex dynamical processes in matter by x-ray diffraction will be discussed.

Supercontinuum generation in quadratic nonlinear waveguides without quasi-phase matching.

PubMed

Guo, Hairun; Zhou, Binbin; Steinert, Michael; Setzpfandt, Frank; Pertsch, Thomas; Chung, Hung-ping; Chen, Yen-Hung; Bache, Morten

2015-02-15

Supercontinuum generation (SCG) is most efficient when the solitons can be excited directly at the pump laser wavelength. Quadratic nonlinear waveguides may induce an effective negative Kerr nonlinearity, so temporal solitons can be directly generated in the normal (positive) dispersion regime overlapping with common ultrafast laser wavelengths. There is no need for waveguide dispersion engineering. Here, we experimentally demonstrate SCG in standard lithium niobate (LN) waveguides without quasi-phase matching (QPM), pumped with femtosecond pulses in the normal dispersion regime. The observed large bandwidths (even octave spanning), together with other experimental data, indicate that negative nonlinearity solitons are indeed excited, which is backed up by numerical simulations. The QPM-free design reduces production complexity, extends the maximum waveguide length, and limits undesired spectral resonances. Finally, nonlinear crystals can be used where QPM is inefficient or impossible, which is important for mid-IR SCG. QPM-free waveguides in mid-IR nonlinear crystals can support negative nonlinearity solitons, as these waveguides have a normal dispersion at the emission wavelengths of mid-IR ultrafast lasers.

On the dynamical nature of the active center in a single-site photocatalyst visualized by 4D ultrafast electron microscopy

PubMed Central

Yoo, Byung-Kuk; Su, Zixue; Thomas, John Meurig; Zewail, Ahmed H.

2016-01-01

Understanding the dynamical nature of the catalytic active site embedded in complex systems at the atomic level is critical to developing efficient photocatalytic materials. Here, we report, using 4D ultrafast electron microscopy, the spatiotemporal behaviors of titanium and oxygen in a titanosilicate catalytic material. The observed changes in Bragg diffraction intensity with time at the specific lattice planes, and with a tilted geometry, provide the relaxation pathway: the Ti4+=O2− double bond transformation to a Ti3+−O1− single bond via the individual atomic displacements of the titanium and the apical oxygen. The dilation of the double bond is up to 0.8 Å and occurs on the femtosecond time scale. These findings suggest the direct catalytic involvement of the Ti3+−O1− local structure, the significance of nonthermal processes at the reactive site, and the efficient photo-induced electron transfer that plays a pivotal role in many photocatalytic reactions. PMID:26729878

Effects of surface nanostructuring and impurity doping on ultrafast carrier dynamics of silicon photovoltaic cells: a pump-probe study

NASA Astrophysics Data System (ADS)

Chen, Tianyu; Nam, Yoon-Ho; Wang, Xinke; Han, Peng; Sun, Wenfeng; Feng, Shengfei; Ye, Jiasheng; Song, Jae-Won; Lee, Jung-Ho; Zhang, Chao; Zhang, Yan

2018-01-01

We present femtosecond optical pump-terahertz probe studies on the ultrafast dynamical processes of photo-generated charge carriers in silicon photovoltaic cells with various nanostructured surfaces and doping densities. The pump-probe measurements provide direct insight on the lifetime of photo-generated carriers, frequency-dependent complex dielectric response along with photoconductivity of silicon photovoltaic cells excited by optical pump pulses. A lifetime of photo-generated carriers of tens of nanosecond is identified from the time-dependent pump-induced attenuation of the terahertz transmission. In addition, we find a large value of the imaginary part of the dielectric function and of the real part of the photoconductivity in silicon photovoltaic cells with micron length nanowires. We attribute these findings to the result of defect-enhanced electron-photon interactions. Moreover, doping densities of phosphorous impurities in silicon photovoltaic cells are also quantified using the Drude-Smith model with our measured frequency-dependent complex photoconductivities.

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.

Two-colour hard X-ray free-electron laser with wide tunability.

PubMed

Hara, Toru; Inubushi, Yuichi; Katayama, Tetsuo; Sato, Takahiro; Tanaka, Hitoshi; Tanaka, Takashi; Togashi, Tadashi; Togawa, Kazuaki; Tono, Kensuke; Yabashi, Makina; Ishikawa, Tetsuya

2013-01-01

Ultrabrilliant, femtosecond X-ray pulses from X-ray free-electron lasers (XFELs) have promoted the investigation of exotic interactions between intense X-rays and matters, and the observation of minute targets with high spatio-temporal resolution. Although a single X-ray beam has been utilized for these experiments, the use of multiple beams with flexible and optimum beam parameters should drastically enhance the capability and potentiality of XFELs. Here we show a new light source of a two-colour double-pulse (TCDP) XFEL in hard X-rays using variable-gap undulators, which realizes a large and flexible wavelength separation of more than 30% with an ultraprecisely controlled time interval in the attosecond regime. Together with sub-10-fs pulse duration and multi-gigawatt peak powers, the TCDP scheme enables us to elucidate X-ray-induced ultrafast transitions of electronic states and structures, which will significantly contribute to the advancement of ultrafast chemistry, plasma and astronomical physics, and quantum X-ray optics.

A dynamic and ultrafast group delay tuning mechanism in two microcavities side-coupled with a waveguide system

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

Wang, Boyun; Wang, Tao, E-mail: wangtao@hust.edu.cn; Tang, Jian

2014-10-07

We theoretically propose a dynamic and ultrafast group delay tuning mechanism in two microcavities side-coupled to a waveguide system through external optical pump beams. The optical Kerr effect modulation method is applied to improve tuning rate with response time of subpicoseconds or even femtoseconds. The group delay of an all-optical analog to electromagnetically induced transparency effect can be controlled by tuning either the frequency of photonic crystal microcavities or the propagation phase of line waveguide. Group delay is controlled between 5.88 and 70.98 ps by dynamically tuning resonant frequencies of the microcavities. Alternatively, the group delay is controlled between 1.86more » and 12.08 ps by dynamically tuning the propagation phase of line waveguide. All observed schemes are analyzed rigorously through finite-difference time-domain simulations and coupled-mode formalism. Results show a new direction toward microstructure integration optical pulse trapping and all-optical dynamical storage of light devices in optical communication and quantum information processing.« 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.

Anisotropic ultrafast response of MoS2 on rippled substrates

NASA Astrophysics Data System (ADS)

Cinquanta, Eugenio; Camellini, Andrea; Martella, Christian; Mennucci, Carlo; Lamperti, Alessio; Della Valle, Giuseppe; Zavelani Rossi, Margherita; Buatier de Mongeot, Francesco; Molle, Alessandro; Stagira, Salvatore

TMDs represent one of the most promising option for new devices characterized by high performances for opto- and nanoelectronics applications. Top-down schemes have been fruitfully exploited for the tuning of TMDs physics by stain engineering in exfoliated flakes. We propose an original bottom-up strategy based on the CVD growth of MoS2 on anisotropic substrates and its characterization by means of pump-probe spectroscopy. The ultrafast response of the rippled MoS2 reveals strongly anisotropic. While the transient absorption emerges as independent from the orientation of the pump beam polarization, the angle between the probe beam polarization and the ripples induces remarkable effects. Within an orthogonal geometry, both the overall intensity of the transient spectrum and the el-ph scattering decay time are halved while the photo-bleaching at 450 nm is blueshifted with respect to the parallel orientation case. Our results demonstrate that the coupling of TMDs with anisotropic substrates is a promising way for the integration of TMDs photonics devices.

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

DOE PAGES

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung; ...

2017-05-24

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

Stacking order dynamics in the quasi-two-dimensional dichalcogenide 1T-TaS2 probed with MeV ultrafast electron diffraction.

PubMed

Le Guyader, L; Chase, T; Reid, A H; Li, R K; Svetin, D; Shen, X; Vecchione, T; Wang, X J; Mihailovic, D; Dürr, H A

2017-07-01

Transitions between different charge density wave (CDW) states in quasi-two-dimensional materials may be accompanied also by changes in the inter-layer stacking of the CDW. Using MeV ultrafast electron diffraction, the out-of-plane stacking order dynamics in the quasi-two-dimensional dichalcogenide 1 T -TaS 2 is investigated for the first time. From the intensity of the CDW satellites aligned around the commensurate l  = 1/6 characteristic stacking order, it is found out that this phase disappears with a 0.3 ps time constant. Simultaneously, in the same experiment, the emergence of the incommensurate phase, with a slightly slower 2.0 ps time constant, is determined from the intensity of the CDW satellites aligned around the incommensurate l  = 1/3 characteristic stacking order. These results might be of relevance in understanding the metallic character of the laser-induced metastable "hidden" state recently discovered in this compound.

Stacking order dynamics in the quasi-two-dimensional dichalcogenide 1 T-TaS 2 probed with MeV ultrafast electron diffraction

DOE PAGES

Le Guyader, L.; Chase, T.; Reid, A. H.; ...

2017-05-03

Transitions between different charge density wave (CDW) states in quasi-two-dimensional materials may be accompanied also by changes in the inter-layer stacking of the CDW. Using MeV ultrafast electron diffraction, the out-of-plane stacking order dynamics in the quasi-two-dimensional dichalcogenide 1 T-TaS 2 is investigated for the first time. From the intensity of the CDW satellites aligned around the commensurate l = 1/6 characteristic stacking order, it is found out that this phase disappears with a 0.3 ps time constant. Simultaneously, in the same experiment, the emergence of the incommensurate phase, with a slightly slower 2.0 ps time constant, is determined frommore » the intensity of the CDW satellites aligned around the incommensurate l = 1/3 characteristic stacking order. Finally, these results might be of relevance in understanding the metallic character of the laser-induced metastable “hidden” state recently discovered in this compound.« less

Ultra-fast Object Recognition from Few Spikes

DTIC Science & Technology

2005-07-06

Computer Science and Artificial Intelligence Laboratory Ultra-fast Object Recognition from Few Spikes Chou Hung, Gabriel Kreiman , Tomaso Poggio...neural code for different kinds of object-related information. *The authors, Chou Hung and Gabriel Kreiman , contributed equally to this work...Supplementary Material is available at http://ramonycajal.mit.edu/ kreiman /resources/ultrafast

Ultrafast Laser System for Producing on-Demand Single-and Multi-Photon Quantum States

DTIC Science & Technology

2015-09-20

14-Mar-2015 Approved for Public Release; Distribution Unlimited Final Report: Ultrafast laser system for producing on-demand single- and multi...Champaign, IL 61820 -7406 14-Mar-2015 ABSTRACT Number of Papers published in peer-reviewed journals: Final Report: Ultrafast laser system for producing

Ultrafast electron diffraction with megahertz MeV electron pulses from a superconducting radio-frequency photoinjector

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

Feng, L. W.; Lin, L.; Huang, S. L.

We report ultrafast relativistic electron diffraction operating at the megahertz repetition rate where the electron beam is produced in a superconducting radio-frequency (rf) photoinjector. We show that the beam quality is sufficiently high to provide clear diffraction patterns from gold and aluminium samples. With the number of electrons, several orders of magnitude higher than that from a normal conducting photocathode rf gun, such high repetition rate ultrafast MeV electron diffraction may open up many new opportunities in ultrafast science.

Ultrafast Photodetection in the Quantum Wells of Single AlGaAs/GaAs-Based Nanowires.

PubMed

Erhard, N; Zenger, S; Morkötter, S; Rudolph, D; Weiss, M; Krenner, H J; Karl, H; Abstreiter, G; Finley, J J; Koblmüller, G; Holleitner, A W

2015-10-14

We investigate the ultrafast optoelectronic properties of single Al0.3Ga0.7As/GaAs core-shell nanowires. The nanowires contain GaAs-based quantum wells. For a resonant excitation of the quantum wells, we find a picosecond photocurrent which is consistent with an ultrafast lateral expansion of the photogenerated charge carriers. This Dember-effect does not occur for an excitation of the GaAs-based core of the nanowires. Instead, the core exhibits an ultrafast displacement current and a photothermoelectric current at the metal Schottky contacts. Our results uncover the optoelectronic dynamics in semiconductor core-shell nanowires comprising quantum wells, and they demonstrate the possibility to use the low-dimensional quantum well states therein for ultrafast photoswitches and photodetectors.

Simple and robust generation of ultrafast laser pulse trains using polarization-independent parallel-aligned thin films

NASA Astrophysics Data System (ADS)

Wang, Andong; Jiang, Lan; Li, Xiaowei; Wang, Zhi; Du, Kun; Lu, Yongfeng

2018-05-01

Ultrafast laser pulse temporal shaping has been widely applied in various important applications such as laser materials processing, coherent control of chemical reactions, and ultrafast imaging. However, temporal pulse shaping has been limited to only-in-lab technique due to the high cost, low damage threshold, and polarization dependence. Herein we propose a novel design of ultrafast laser pulse train generation device, which consists of multiple polarization-independent parallel-aligned thin films. Various pulse trains with controllable temporal profile can be generated flexibly by multi-reflections within the splitting films. Compared with other pulse train generation techniques, this method has advantages of compact structure, low cost, high damage threshold and polarization independence. These advantages endow it with high potential for broad utilization in ultrafast applications.

Space charge effects in ultrafast electron diffraction and imaging

NASA Astrophysics Data System (ADS)

Tao, Zhensheng; Zhang, He; Duxbury, P. M.; Berz, Martin; Ruan, Chong-Yu

2012-02-01

Understanding space charge effects is central for the development of high-brightness ultrafast electron diffraction and microscopy techniques for imaging material transformation with atomic scale detail at the fs to ps timescales. We present methods and results for direct ultrafast photoelectron beam characterization employing a shadow projection imaging technique to investigate the generation of ultrafast, non-uniform, intense photoelectron pulses in a dc photo-gun geometry. Combined with N-particle simulations and an analytical Gaussian model, we elucidate three essential space-charge-led features: the pulse lengthening following a power-law scaling, the broadening of the initial energy distribution, and the virtual cathode threshold. The impacts of these space charge effects on the performance of the next generation high-brightness ultrafast electron diffraction and imaging systems are evaluated.

Quantum Zeno Blockade for Next Generation Optical Switching in Fiber Systems

DTIC Science & Technology

2013-09-01

and utilized a self - referential quantum process tomography method to observe the Zeno effect in optical fiber using the ultrafast all- optical switch...controllable and can be used as a knob to study the core physics behind the Zeno-based switching. For this experiment, we developed a self - referential ...efficient optical communications. The quantum Zeno effect can be used to induce or inhibit optical switching through a variety of processes , all of