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

PubMed

Stingel, Ashley M; Petersen, Poul B

2018-03-15

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

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.

A general strategy for the ultrafast surface modification of metals.

PubMed

Shen, Mingli; Zhu, Shenglong; Wang, Fuhui

2016-12-07

Surface modification is an essential step in engineering materials that can withstand the increasingly aggressive environments encountered in various modern energy-conversion systems and chemical processing industries. However, most traditional technologies exhibit disadvantages such as slow diffusion kinetics, processing difficulties or compatibility issues. Here, we present a general strategy for the ultrafast surface modification of metals inspired by electromigration, using aluminizing austenitic stainless steel as an example. Our strategy facilitates the rapid formation of a favourable ductile surface layer composed of FeCrAl or β-FeAl within only 10 min compared with several hours in conventional processes. This result indicates that electromigration can be used to achieve the ultrafast surface modification of metals and can overcome the limitations of traditional technologies. This strategy could be used to aluminize ultra-supercritical steam tubing to withstand aggressive oxidizing environments.

A general strategy for the ultrafast surface modification of metals

PubMed Central

Shen, Mingli; Zhu, Shenglong; Wang, Fuhui

2016-01-01

Surface modification is an essential step in engineering materials that can withstand the increasingly aggressive environments encountered in various modern energy-conversion systems and chemical processing industries. However, most traditional technologies exhibit disadvantages such as slow diffusion kinetics, processing difficulties or compatibility issues. Here, we present a general strategy for the ultrafast surface modification of metals inspired by electromigration, using aluminizing austenitic stainless steel as an example. Our strategy facilitates the rapid formation of a favourable ductile surface layer composed of FeCrAl or β-FeAl within only 10 min compared with several hours in conventional processes. This result indicates that electromigration can be used to achieve the ultrafast surface modification of metals and can overcome the limitations of traditional technologies. This strategy could be used to aluminize ultra-supercritical steam tubing to withstand aggressive oxidizing environments. PMID:27924909

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.

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.

Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate

DOE PAGES

Coslovich, Giacomo; Kemper, Alexander F.; Behl, Sascha; ...

2017-11-24

The ability to probe symmetry-breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-terahertz response of the model stripe compound La 1.75Sr 0.25NiO 4, yielding novel insight into its electronic and structural dynamics following an ultrafast opticalmore » quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen—as witnessed by time-delayed suppression of zone-folded Ni–O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. As a result, the hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry-breaking dynamics in solids.« less

Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate

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

Coslovich, Giacomo; Kemper, Alexander F.; Behl, Sascha

The ability to probe symmetry-breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-terahertz response of the model stripe compound La 1.75Sr 0.25NiO 4, yielding novel insight into its electronic and structural dynamics following an ultrafast opticalmore » quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen—as witnessed by time-delayed suppression of zone-folded Ni–O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. As a result, the hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry-breaking dynamics in solids.« less

Femtosecond coherent nuclear dynamics of excited tetraphenylethylene: Ultrafast transient absorption and ultrafast Raman loss spectroscopic studies

NASA Astrophysics Data System (ADS)

Kayal, Surajit; Roy, Khokan; Umapathy, Siva

2018-01-01

Ultrafast torsional dynamics plays an important role in the photoinduced excited state dynamics. Tetraphenylethylene (TPE), a model system for the molecular motor, executes interesting torsional dynamics upon photoexcitation. The photoreaction of TPE involves ultrafast internal conversion via a nearly planar intermediate state (relaxed state) that further leads to a twisted zwitterionic state. Here, we report the photoinduced structural dynamics of excited TPE during the course of photoisomerization in the condensed phase by ultrafast Raman loss (URLS) and femtosecond transient absorption (TA) spectroscopy. TA measurements on the S1 state reveal step-wise population relaxation from the Franck-Condon (FC) state → relaxed state → twisted state, while the URLS study provides insights on the vibrational dynamics during the course of the reaction. The TA spectral dynamics and vibrational Raman amplitudes within 1 ps reveal vibrational wave packet propagating from the FC state to the relaxed state. Fourier transformation of this oscillation leads to a ˜130 cm-1 low-frequency phenyl torsional mode. Two vibrational marker bands, Cet=Cet stretching (˜1512 cm-1) and Cph=Cph stretching (˜1584 cm-1) modes, appear immediately after photoexcitation in the URLS spectra. The initial red-shift of the Cph=Cph stretching mode with a time constant of ˜400 fs (in butyronitrile) is assigned to the rate of planarization of excited TPE. In addition, the Cet=Cet stretching mode shows initial blue-shift within 1 ps followed by frequency red-shift, suggesting that on the sub-picosecond time scale, structural relaxation is dominated by phenyl torsion rather than the central Cet=Cet twist. Furthermore, the effect of the solvent on the structural dynamics is discussed in the context of ultrafast nuclear dynamics and solute-solvent coupling.

Femtosecond coherent nuclear dynamics of excited tetraphenylethylene: Ultrafast transient absorption and ultrafast Raman loss spectroscopic studies.

PubMed

Kayal, Surajit; Roy, Khokan; Umapathy, Siva

2018-01-14

Ultrafast torsional dynamics plays an important role in the photoinduced excited state dynamics. Tetraphenylethylene (TPE), a model system for the molecular motor, executes interesting torsional dynamics upon photoexcitation. The photoreaction of TPE involves ultrafast internal conversion via a nearly planar intermediate state (relaxed state) that further leads to a twisted zwitterionic state. Here, we report the photoinduced structural dynamics of excited TPE during the course of photoisomerization in the condensed phase by ultrafast Raman loss (URLS) and femtosecond transient absorption (TA) spectroscopy. TA measurements on the S 1 state reveal step-wise population relaxation from the Franck-Condon (FC) state → relaxed state → twisted state, while the URLS study provides insights on the vibrational dynamics during the course of the reaction. The TA spectral dynamics and vibrational Raman amplitudes within 1 ps reveal vibrational wave packet propagating from the FC state to the relaxed state. Fourier transformation of this oscillation leads to a ∼130 cm -1 low-frequency phenyl torsional mode. Two vibrational marker bands, C et =C et stretching (∼1512 cm -1 ) and C ph =C ph stretching (∼1584 cm -1 ) modes, appear immediately after photoexcitation in the URLS spectra. The initial red-shift of the C ph =C ph stretching mode with a time constant of ∼400 fs (in butyronitrile) is assigned to the rate of planarization of excited TPE. In addition, the C et =C et stretching mode shows initial blue-shift within 1 ps followed by frequency red-shift, suggesting that on the sub-picosecond time scale, structural relaxation is dominated by phenyl torsion rather than the central C et =C et twist. Furthermore, the effect of the solvent on the structural dynamics is discussed in the context of ultrafast nuclear dynamics and solute-solvent coupling.

Ultra-fast boriding of metal surfaces for improved properties

DOEpatents

Timur, Servet; Kartal, Guldem; Eryilmaz, Osman L.; Erdemir, Ali

2015-02-10

A method of ultra-fast boriding of a metal surface. The method includes the step of providing a metal component, providing a molten electrolyte having boron components therein, providing an electrochemical boriding system including an induction furnace, operating the induction furnace to establish a high temperature for the molten electrolyte, and boriding the metal surface to achieve a boride layer on the metal surface.

Effectively Single-Mode Self-Recovering Ultrafast Nonlinear Nanowire Surface Plasmons

NASA Astrophysics Data System (ADS)

Tuniz, Alessandro; Weidlich, Stefan; Schmidt, Markus A.

2018-04-01

We report on a regime for surface-plasmon propagation, which is robust to defects and effectively single mode, and we exploit it for accessing the ultrafast nonlinear response of gold on centimeter-long subwavelength-diameter cylindrical nanowires. The hybrid plasmonic-photonic platform is formed by a gold nanowire, monolithically integrated into the core of an optical fiber. We show that, despite the dual-waveguide nature of this structure, the long-range surface plasmon is the only effectively propagating mode in the near infrared, which self-recovers in the presence of gaps via a light-recapturing effect. This self-recovery overcomes detrimental effects of wire discontinuities and enables measurements of the ultrafast nonlinearity of gold, which we perform for a 28-fs pulse duration.

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.

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.

Probing Ultrafast Electron Dynamics at Surfaces Using Soft X-Ray Transient Reflectivity Spectroscopy

NASA Astrophysics Data System (ADS)

Baker, L. Robert; Husek, Jakub; Biswas, Somnath; Cirri, Anthony

The ability to probe electron dynamics with surface sensitivity on the ultrafast time scale is critical for understanding processes such as charge separation, injection, and surface trapping that mediate efficiency in catalytic and energy conversion materials. Toward this goal, we have developed a high harmonic generation (HHG) light source for femtosecond soft x-ray reflectivity. Using this light source we investigated the ultrafast carrier dynamics at the surface of single crystalline α-Fe2O3, polycrystalline α-Fe2O3, and the mixed metal oxide, CuFeO2. We have recently demonstrated that CuFeO2 in particular is a selective catalyst for photo-electrochemical CO2 reduction to acetate; however, the role of electronic structure and charge carrier dynamics in mediating catalytic selectivity has not been well understood. Soft x-ray reflectivity measurements probe the M2,3, edges of the 3d transition metals, which provide oxidation and spin state resolution with element specificity. In addition to chemical state specificity, these measurements are also surface sensitive, and by independently simulating the contributions of the real and imaginary components of the complex refractive index, we can differentiate between surface and sub-surface contributions to the excited state spectrum. Accordingly, this work demonstrates the ability to probe ultrafast carrier dynamics in catalytic materials with element and chemical state specificity and with surface sensitivity.

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

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

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

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

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.

Communication: Probing non-equilibrium vibrational relaxation pathways of highly excited C≡N stretching modes following ultrafast back-electron transfer.

PubMed

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

2012-06-28

Fifth-order nonlinear visible-infrared spectroscopy is used to probe coherent and incoherent vibrational energy relaxation dynamics of highly excited vibrational modes indirectly populated via ultrafast photoinduced back-electron transfer in a trinuclear cyano-bridged mixed-valence complex. The flow of excess energy deposited into four C≡N stretching (ν(CN)) modes of the molecule is monitored by performing an IR pump-probe experiment as a function of the photochemical reaction (τ(vis)). Our results provide experimental evidence that the nuclear motions of the molecule are both coherently and incoherently coupled to the electronic charge transfer process. We observe that intramolecular vibrational relaxation dynamics among the highly excited ν(CN) modes change significantly en route to equilibrium. The experiment also measures a 7 cm(-1) shift in the frequency of a ∼57 cm(-1) oscillation reflecting a modulation of the coupling between the probed high-frequency ν(CN) modes for τ(vis) < 500 fs.

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

PubMed

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

2017-08-03

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

Polycrystallinity of Lithographically Fabricated Plasmonic Nanostructures Dominates Their Acoustic Vibrational Damping.

PubMed

Yi, Chongyue; Su, Man-Nung; Dongare, Pratiksha D; Chakraborty, Debadi; Cai, Yi-Yu; Marolf, David M; Kress, Rachael N; Ostovar, Behnaz; Tauzin, Lawrence J; Wen, Fangfang; Chang, Wei-Shun; Jones, Matthew R; Sader, John E; Halas, Naomi J; Link, Stephan

2018-06-13

The study of acoustic vibrations in nanoparticles provides unique and unparalleled insight into their mechanical properties. Electron-beam lithography of nanostructures allows precise manipulation of their acoustic vibration frequencies through control of nanoscale morphology. However, the dissipation of acoustic vibrations in this important class of nanostructures has not yet been examined. Here we report, using single-particle ultrafast transient extinction spectroscopy, the intrinsic damping dynamics in lithographically fabricated plasmonic nanostructures. We find that in stark contrast to chemically synthesized, monocrystalline nanoparticles, acoustic energy dissipation in lithographically fabricated nanostructures is solely dominated by intrinsic damping. A quality factor of Q = 11.3 ± 2.5 is observed for all 147 nanostructures, regardless of size, geometry, frequency, surface adhesion, and mode. This result indicates that the complex Young's modulus of this material is independent of frequency with its imaginary component being approximately 11 times smaller than its real part. Substrate-mediated acoustic vibration damping is strongly suppressed, despite strong binding between the glass substrate and Au nanostructures. We anticipate that these results, characterizing the optomechanical properties of lithographically fabricated metal nanostructures, will help inform their design for applications such as photoacoustic imaging agents, high-frequency resonators, and ultrafast optical switches.

Ultrafast fragmentation dynamics of triply charged carbon dioxide: Vibrational-mode-dependent molecular bond breakage

NASA Astrophysics Data System (ADS)

Yang, HongJiang; Wang, Enliang; Dong, WenXiu; Gong, Maomao; Shen, Zhenjie; Tang, Yaguo; Shan, Xu; Chen, Xiangjun

2018-05-01

The a b i n i t i o molecular dynamics (MD) simulations using an atom-centered density matrix propagation method have been carried out to investigate the fragmentation of the ground-state triply charged carbon dioxide, CO23 +→C+ + Oa+ + Ob+ . Ten thousands of trajectories have been simulated. By analyzing the momentum correlation of the final fragments, it is demonstrated that the sequential fragmentation dominates in the three-body dissociation, consistent with our experimental observations which were performed by electron collision at impact energy of 1500 eV. Furthermore, the MD simulations allow us to have detailed insight into the ultrafast evolution of the molecular bond breakage at a very early stage, within several tens of femtoseconds, and the result shows that the initial nuclear vibrational mode plays a decisive role in switching the dissociation pathways.

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.

Surface acoustic wave (SAW) vibration sensors.

PubMed

Filipiak, Jerzy; Solarz, Lech; Steczko, Grzegorz

2011-01-01

In the paper a feasibility study on the use of surface acoustic wave (SAW) vibration sensors for electronic warning systems is presented. The system is assembled from concatenated SAW vibration sensors based on a SAW delay line manufactured on a surface of a piezoelectric plate. Vibrations of the plate are transformed into electric signals that allow identification of the sensor and localization of a threat. The theoretical study of sensor vibrations leads us to the simple isotropic model with one degree of freedom. This model allowed an explicit description of the sensor plate movement and identification of the vibrating sensor. Analysis of frequency response of the ST-cut quartz sensor plate and a damping speed of its impulse response has been conducted. The analysis above was the basis to determine the ranges of parameters for vibrating plates to be useful in electronic warning systems. Generally, operation of electronic warning systems with SAW vibration sensors is based on the analysis of signal phase changes at the working frequency of delay line after being transmitted via two circuits of concatenated four-terminal networks. Frequencies of phase changes are equal to resonance frequencies of vibrating plates of sensors. The amplitude of these phase changes is proportional to the amplitude of vibrations of a sensor plate. Both pieces of information may be sent and recorded jointly by a simple electrical unit.

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

PubMed

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

2018-04-24

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

Vibrational relaxation in liquid chloroform following ultrafast excitation of the CH stretch fundamental

NASA Astrophysics Data System (ADS)

Sibert, Edwin L.; Rey, Rossend

2002-01-01

Vibrational energy flow in liquid chloroform that follows the ultrafast excitation of the CH stretch fundamental is modeled using semiclassical methods. Relaxation rates are calculated using Landau-Teller theory and a time-dependent method both of which consider a quantum mechanical CHCl3 solute molecule coupled to a classical bath of CHCl3 solvent molecules. Probability flow is examined for several potentials to determine the sensitivity of calculated relaxation rates to the parameters that describe the model potentials. Three stages of relaxation are obtained. Probability is calculated to decay initially to a single acceptor state, a combination state of the solute molecule with two quanta of excitation in the CH bend and one in the CCl stretch, in 13-23 ps depending on the potential model employed. This is followed by rapid and complex intramolecular energy flow into the remaining vibrational degrees of freedom. During this second stage the lowest frequency Cl-C-Cl bend is found to serve as a conduit for energy loss to the solvent. The bottleneck for relaxation back to the ground state is predicted to be the slow 100-200 ps relaxation of the CH bend and CCl stretch fundamentals. Several aspects of the incoherent anti-Stokes scattering that follows strong infrared excitation of the CH fundamental as observed by Graener, Zürl, and Hoffman [J. Phys. Chem. B 101, 1745 (1997)] are elucidated in the present study.

Ultrafast vibrational dynamics of BH{sub 4}{sup −} ions in liquid and crystalline environments

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

Tyborski, Tobias, E-mail: tyborski@mbi-berlin.de; Costard, Rene; Woerner, Michael

2014-07-21

Ultrafast vibrational dynamics of BH{sub 4}{sup −} ions, the key units in boron hydride materials for hydrogen storage, are studied in diluted polar liquid solution and in NaBH{sub 4} crystallites by femtosecond infrared spectroscopy. Two-color pump-probe experiments reveal v = 1 lifetimes of 3 ps for the asymmetric BH{sub 4}{sup −} stretching mode ν{sub 3} and of 3.6 ps for the asymmetric bending mode ν{sub 4} in the solvent isopropylamine. We provide direct evidence for the BH{sub 4}{sup −} stretching relaxation pathway via the asymmetric bending mode ν{sub 4} by probing the latter after femtosecond excitation of ν{sub 3}. Pump-probemore » traces measured in the crystalline phase show signatures of radiative coupling between the densely packed BH{sub 4}{sup −} oscillators, most clearly manifested in an accelerated subpicosecond depopulation of the v = 1 state of the ν{sub 4} mode. The radiative decay is followed by incoherent vibrational relaxation similar to the liquid phase. The excess energy released in the relaxation processes of the BH{sub 4}{sup −} intramolecular modes is transferred into the environment with thermal pump-probe signals being much more pronounced in the dense solid than in the diluted solution.« less

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

PubMed

Dombi, Péter; Rácz, Péter

2008-03-03

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

Vibrational Action Spectroscopy of Solids: New Surface-Sensitive Technique

NASA Astrophysics Data System (ADS)

Wu, Zongfang; Płucienik, Agata; Feiten, Felix E.; Naschitzki, Matthias; Wachsmann, Walter; Gewinner, Sandy; Schöllkopf, Wieland; Staemmler, Volker; Kuhlenbeck, Helmut; Freund, Hans-Joachim

2017-09-01

Vibrational action spectroscopy employing infrared radiation from a free-electron laser has been successfully used for many years to study the vibrational and structural properties of gas phase aggregates. Despite the high sensitivity of this method no relevant studies have yet been conducted for solid sample surfaces. We have set up an experiment for the application of this method to such targets, using infrared light from the free-electron laser of the Fritz Haber Institute. In this Letter, we present first results of this technique with adsorbed argon and neon atoms as messengers. We were able to detect surface-located vibrations of a thin V2O3(0 0 0 1 ) film on Au(111) as well as adsorbate vibrations, demonstrating that this method is highly surface sensitive. We consider that the dominant channel for desorption of the messenger atoms is direct inharmonic vibrational coupling, which is essentially insensitive to subsurface or bulk vibrations. Another channel is thermal desorption due to sample heating by absorption of infrared light. The high surface sensitivity of the nonthermal channel and its insensitivity to subsurface modes makes this technique an ideal tool for the study of surface-located vibrations.

Vibrational Action Spectroscopy of Solids: New Surface-Sensitive Technique.

PubMed

Wu, Zongfang; Płucienik, Agata; Feiten, Felix E; Naschitzki, Matthias; Wachsmann, Walter; Gewinner, Sandy; Schöllkopf, Wieland; Staemmler, Volker; Kuhlenbeck, Helmut; Freund, Hans-Joachim

2017-09-29

Vibrational action spectroscopy employing infrared radiation from a free-electron laser has been successfully used for many years to study the vibrational and structural properties of gas phase aggregates. Despite the high sensitivity of this method no relevant studies have yet been conducted for solid sample surfaces. We have set up an experiment for the application of this method to such targets, using infrared light from the free-electron laser of the Fritz Haber Institute. In this Letter, we present first results of this technique with adsorbed argon and neon atoms as messengers. We were able to detect surface-located vibrations of a thin V_{2}O_{3}(0001) film on Au(111) as well as adsorbate vibrations, demonstrating that this method is highly surface sensitive. We consider that the dominant channel for desorption of the messenger atoms is direct inharmonic vibrational coupling, which is essentially insensitive to subsurface or bulk vibrations. Another channel is thermal desorption due to sample heating by absorption of infrared light. The high surface sensitivity of the nonthermal channel and its insensitivity to subsurface modes makes this technique an ideal tool for the study of surface-located vibrations.

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.

Mixed quantum-classical simulations of the vibrational relaxation of photolyzed carbon monoxide in a hemoprotein

NASA Astrophysics Data System (ADS)

Schubert, Alexander; Falvo, Cyril; Meier, Christoph

2016-08-01

We present mixed quantum-classical simulations on relaxation and dephasing of vibrationally excited carbon monoxide within a protein environment. The methodology is based on a vibrational surface hopping approach treating the vibrational states of CO quantum mechanically, while all remaining degrees of freedom are described by means of classical molecular dynamics. The CO vibrational states form the "surfaces" for the classical trajectories of protein and solvent atoms. In return, environmentally induced non-adiabatic couplings between these states cause transitions describing the vibrational relaxation from first principles. The molecular dynamics simulation yields a detailed atomistic picture of the energy relaxation pathways, taking the molecular structure and dynamics of the protein and its solvent fully into account. Using the ultrafast photolysis of CO in the hemoprotein FixL as an example, we study the relaxation of vibrationally excited CO and evaluate the role of each of the FixL residues forming the heme pocket.

The vibrational Jahn-Teller effect in E⊗e systems

NASA Astrophysics Data System (ADS)

Thapaliya, Bishnu P.; Dawadi, Mahesh B.; Ziegler, Christopher; Perry, David S.

2015-10-01

The Jahn-Teller theorem is applied in the vibrational context where degenerate high-frequency vibrational states (E) are considered as adiabatic functions of low-frequency vibrational coordinates (e). For CH3CN and Cr(C6H6)(CO)3, the global minimum of the non-degenerate electronic potential energy surface occurs at the C3v geometry, but in CH3OH, the equilibrium geometry is far from the C3v reference geometry. In the former cases, the computed spontaneous Jahn-Teller distortion is exceptionally small. In methanol, the vibrational Jahn-Teller interaction results in the splitting of the degenerate E-type CH stretch into what have been traditionally assigned as the distinct ν2 and ν9 vibrational bands. The ab initio vibrational frequencies are fit precisely by a two-state high-order Jahn-Teller Hamiltonian (Viel and Eisfeld, 2004). The presence of vibrational conical intersections, including 7 for CH3OH, has implications for spectroscopy, for geometric phase, and for ultrafast localized non-adiabatic energy transfer.

Imaging CF3I conical intersection and photodissociation dynamics by ultrafast electron diffraction

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

Yang, Jie

Conical intersections play a critical role in excited state dynamics of polyatomic molecules, as they govern the reaction pathways of many nonadiabatic processes. However, ultrafast probes have lacked sufficient spatial resolution to image wavepacket trajectories through these intersections directly. Here we present the simultaneous experimental characterization of one-photon and two-photon excitation channels in isolated CF3I molecules using ultrafast gas phase electron diffraction. In the two-photon channel, we have mapped out the real space trajectories of a coherent nuclear wavepacket, which bifurcates onto two potential energy surfaces when passing through a conical intersection. In the one-photon channel, we have resolved excitationmore » of both the umbrella and the breathing vibrational modes in the CF3 fragment in multiple nuclear dimensions. These findings benchmark and validate ab-initio nonadiabatic dynamics calculations.« less

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.

Structural dynamics of surfaces by ultrafast electron crystallography: experimental and multiple scattering theory.

PubMed

Schäfer, Sascha; Liang, Wenxi; Zewail, Ahmed H

2011-12-07

Recent studies in ultrafast electron crystallography (UEC) using a reflection diffraction geometry have enabled the investigation of a wide range of phenomena on the femtosecond and picosecond time scales. In all these studies, the analysis of the diffraction patterns and their temporal change after excitation was performed within the kinematical scattering theory. In this contribution, we address the question, to what extent dynamical scattering effects have to be included in order to obtain quantitative information about structural dynamics. We discuss different scattering regimes and provide diffraction maps that describe all essential features of scatterings and observables. The effects are quantified by dynamical scattering simulations and examined by direct comparison to the results of ultrafast electron diffraction experiments on an in situ prepared Ni(100) surface, for which structural dynamics can be well described by a two-temperature model. We also report calculations for graphite surfaces. The theoretical framework provided here allows for further UEC studies of surfaces especially at larger penetration depths and for those of heavy-atom materials. © 2011 American Institute of Physics

PREFACE: Ultrafast biophotonics Ultrafast biophotonics

NASA Astrophysics Data System (ADS)

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

2010-08-01

reduced chromatic aberration effects. These extensive advantages have led to further exploration of nonlinear processes including second-harmonic generation (SHG) microscopy and third-harmonic generation (THG) microscopy. Second-harmonic generation has provided biologists with an extremely powerful tool for generating contrast in biological imaging, with the additional benefit of non-invasive three-dimensional imaging. The recent popularity of THG microscopy is largely due to the fact that three-dimensional imaging is achievable without the need for any labels, but rather relying on the intrinsic properties of the biological specimen itself. This optical nonlinear technique has attracted much attention recently from the biological community due to its non-invasive capabilities. Users of ultrafast lasers in the biological and medical fields are becoming a fast-growing community, employing pulse-shaping microscopy, resolution-enhancing microscopy techniques, linear and nonlinear micro-spectroscopy, functional deep-tissue imaging, optical coherence tomography, nonlinear fluorescence microscopy, molecular imaging and control, harmonic microscopy and femtosecond lifetime imaging, for cutting-edge research concerning the interaction of light with biological dynamics. The adaptability of ultrafast lasers to interact with a large array of materials through nonlinear excitation has enabled precise control of laser fluence allowing for highly localized material interactions, permitting micro-structured fabricated surfaces. The resultant multi-dimensional fabricated micro-structures are capable of replicating and/or manipulating microenvironments for controlled cell biology. In this special issue of Journal of Optics readers have a chance to view a collection of new contributions to the growing research field of ultrafast biophotonics. They are presented with recent advances in ultrafast technology applied to biological and medical investigations, where topics include advances in

Transverse Mode Dynamics and Ultrafast Modulation of Vertical-Cavity Surface-Emitting Lasers

NASA Technical Reports Server (NTRS)

Ning, Cun-Zheng; Biegel, Bryan A. (Technical Monitor)

2002-01-01

We show that multiple transverse mode dynamics of VCSELs (Vertical-Cavity Surface-Emitting Lasers) can be utilized to generate ultrafast intensity modulation at a frequency over 100 GHz, much higher than the relaxation oscillation frequency. Such multimode beating can be greatly enhanced by taking laser output from part of the output facet.

Theoretical study on ultrafast intersystem crossing of chromium(III) acetylacetonate

NASA Astrophysics Data System (ADS)

Ando, Hideo; Iuchi, Satoru; Sato, Hirofumi

2012-05-01

In the relaxation process from the 4T2g state of chromium(III) acetylacetonate, CrIII(acac)3, ultrafast intersystem crossing (ISC) competes with vibrational relaxation (VR). This contradicts the conventional cascade model, where ISC rates are slower than VR ones. We hence investigate the relaxation process with quantum chemical calculations and excited-state wavepacket simulations to obtain clues about the origins of the ultrafast ISC. It is found that a potential energy curve of the 4T2g state crosses those of the 2T1g states near the Franck-Condon region and their spin-orbit couplings are strong. Consequently, ultrafast ISC between these states is observed in the wavepacket simulation.

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.

A direct evidence of vibrationally delocalized response at ice surface.

PubMed

Ishiyama, Tatsuya; Morita, Akihiro

2014-11-14

Surface-specific vibrational spectroscopic responses at isotope diluted ice and amorphous ice are investigated by molecular dynamics (MD) simulations combined with quantum mechanics/molecular mechanics calculations. The intense response specific to the ordinary crystal ice surface is predicted to be significantly suppressed in the isotopically diluted and amorphous ices, demonstrating the vibrational delocalization at the ordinary ice surface. The collective vibration at the ice surface is also analyzed with varying temperature by the MD simulation.

Spatial and temporal ultrafast imaging and control of terahertz wavepackets

NASA Astrophysics Data System (ADS)

Koehl, Richard Michael

Some polar optical phonons couple strongly to far- infrared electromagnetic radiation and move at light-like speeds through dielectric media. These phonon-polaritons retain both ionic and electromagnetic character. One of the fruitful implications of this mixing is that vibrational and electronic nonlinearities in ferroelectric and other highly anharmonic media interact with traveling electromagnetic waves spanning several frequency regimes, permitting nonlinear wave mixing at infrared and optical frequencies. Nonlinear optical mixing techniques are well-developed because optical light is easy to produce, but the lack of similar far- infrared sources has stymied similar efforts at terahertz frequencies. Nonlinear interactions in this frequency regime provide information about vibrational potential energy surfaces and are very strong when the lattice vibration is associated with a phase transition. In this thesis, I review methods based on a well known nonlinear optical technique, impulsive stimulated Raman scattering (ISRS), to monitor the progress of coherent phonon polaritons in a highly nonlinear ferroelectric, lithium tantalate. I also advance multiple-pulse ISRS optical techniques to attempt to elucidate information about the ferroelectric's vibrational potential energy surface, and I discuss significant recent progress that has been made in the development of ultrafast optical tools to generate far-infrared radiation through ISRS at specified times and spatial locations and control the interactions of coherent phonon-polariton wavepackets. (Copies available exclusively from MIT Libraries, Rm. 14-0551, Cambridge, MA 02139-4307. Ph. 617-253-5668; Fax 617-253-1690.)

2D heterodyne-detected sum frequency generation study on the ultrafast vibrational dynamics of H{sub 2}O and HOD water at charged interfaces

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

Inoue, Ken-ichi; Singh, Prashant C.; Nihonyanagi, Satoshi

2015-06-07

Two-dimensional heterodyne-detected vibrational sum-frequency generation (2D HD-VSFG) spectroscopy is applied to study the ultrafast vibrational dynamics of water at positively charged aqueous interfaces, and 2D HD-VSFG spectra of cetyltrimethylammonium bromide (CTAB)/water interfaces in the whole hydrogen-bonded OH stretch region (3000 cm{sup −1} ≤ ω{sub pump} ≤ 3600 cm{sup −1}) are measured. 2D HD-VSFG spectrum of the CTAB/isotopically diluted water (HOD-D{sub 2}O) interface exhibits a diagonally elongated bleaching lobe immediately after excitation, which becomes round with a time constant of ∼0.3 ps due to spectral diffusion. In contrast, 2D HD-VSFG spectrum of the CTAB/H{sub 2}O interface at 0.0 ps clearly showsmore » two diagonal peaks and their cross peaks in the bleaching region, corresponding to the double peaks observed at 3230 cm{sup −1} and 3420 cm{sup −1} in the steady-state HD-VSFG spectrum. Horizontal slices of the 2D spectrum show that the relative intensity of the two peaks of the bleaching at the CTAB/H{sub 2}O interface gradually change with the change of the pump frequency. We simulate the pump-frequency dependence of the bleaching feature using a model that takes account of the Fermi resonance and inhomogeneity of the OH stretch vibration, and the simulated spectra reproduce the essential features of the 2D HD-VSFG spectra of the CTAB/H{sub 2}O interface. The present study demonstrates that heterodyne detection of the time-resolved VSFG is critically important for studying the ultrafast dynamics of water interfaces and for unveiling the underlying mechanism.« less

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.

Imaging surface acoustic wave dynamics in semiconducting polymers by scanning ultrafast electron microscopy.

PubMed

Najafi, Ebrahim; Liao, Bolin; Scarborough, Timothy; Zewail, Ahmed

2018-01-01

Understanding the mechanical properties of organic semiconductors is essential to their electronic and photovoltaic applications. Despite a large volume of research directed toward elucidating the chemical, physical and electronic properties of these materials, little attention has been directed toward understanding their thermo-mechanical behavior. Here, we report the ultrafast imaging of surface acoustic waves (SAWs) on the surface of the Poly(3-hexylthiophene-2,5-diyl) (P3HT) thin film at the picosecond and nanosecond timescales. We then use these images to measure the propagation velocity of SAWs, which we then employ to determine the Young's modulus of P3HT. We further validate our experimental observation by performing a semi-empirical transient thermoelastic finite element analysis. Our findings demonstrate the potential of ultrafast electron microscopy to not only probe charge carrier dynamics in materials as previously reported, but also to measure their mechanical properties with great accuracy. This is particularly important when in situ characterization of stiffness for thin devices and nanomaterials is required. Copyright © 2017 Elsevier B.V. All rights reserved.

Ultrafast electron crystallography: Transient structures of molecules, surfaces, and phase transitions

PubMed Central

Ruan, Chong-Yu; Vigliotti, Franco; Lobastov, Vladimir A.; Chen, Songye; Zewail, Ahmed H.

2004-01-01

The static structure of macromolecular assemblies can be mapped out with atomic-scale resolution by using electron diffraction and microscopy of crystals. For transient nonequilibrium structures, which are critical to the understanding of dynamics and mechanisms, both spatial and temporal resolutions are required; the shortest scales of length (0.1–1 nm) and time (10–13 to 10–12 s) represent the quantum limit, the nonstatistical regime of rates. Here, we report the development of ultrafast electron crystallography for direct determination of structures with submonolayer sensitivity. In these experiments, we use crystalline silicon as a template for different adsorbates: hydrogen, chlorine, and trifluoroiodomethane. We observe the coherent restructuring of the surface layers with subangstrom displacement of atoms after the ultrafast heat impulse. This nonequilibrium dynamics, which is monitored in steps of 2 ps (total change ≤10 ps), contrasts that of the nanometer substrate. The effect of adsorbates and the phase transition at higher fluences were also studied through the evolution of streaks of interferences, Bragg spots (and their rocking curves), and rings in the diffraction patterns. We compare these results with kinematical theory and those of x-ray diffraction developed to study bulk behaviors. The sensitivity achieved here, with the 6 orders of magnitude larger cross section than x-ray diffraction, and with the capabilities of combined spatial (≈0.01 Å) and temporal (300–600 fs) resolutions, promise diverse applications for this ultrafast electron crystallography tabletop methodology. PMID:14745037

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

Scanning ultrafast electron microscopy.

PubMed

Yang, Ding-Shyue; Mohammed, Omar F; Zewail, Ahmed H

2010-08-24

Progress has been made in the development of four-dimensional ultrafast electron microscopy, which enables space-time imaging of structural dynamics in the condensed phase. In ultrafast electron microscopy, the electrons are accelerated, typically to 200 keV, and the microscope operates in the transmission mode. Here, we report the development of scanning ultrafast electron microscopy using a field-emission-source configuration. Scanning of pulses is made in the single-electron mode, for which the pulse contains at most one or a few electrons, thus achieving imaging without the space-charge effect between electrons, and still in ten(s) of seconds. For imaging, the secondary electrons from surface structures are detected, as demonstrated here for material surfaces and biological specimens. By recording backscattered electrons, diffraction patterns from single crystals were also obtained. Scanning pulsed-electron microscopy with the acquired spatiotemporal resolutions, and its efficient heat-dissipation feature, is now poised to provide in situ 4D imaging and with environmental capability.

Scanning ultrafast electron microscopy

PubMed Central

Yang, Ding-Shyue; Mohammed, Omar F.; Zewail, Ahmed H.

2010-01-01

Progress has been made in the development of four-dimensional ultrafast electron microscopy, which enables space-time imaging of structural dynamics in the condensed phase. In ultrafast electron microscopy, the electrons are accelerated, typically to 200 keV, and the microscope operates in the transmission mode. Here, we report the development of scanning ultrafast electron microscopy using a field-emission-source configuration. Scanning of pulses is made in the single-electron mode, for which the pulse contains at most one or a few electrons, thus achieving imaging without the space-charge effect between electrons, and still in ten(s) of seconds. For imaging, the secondary electrons from surface structures are detected, as demonstrated here for material surfaces and biological specimens. By recording backscattered electrons, diffraction patterns from single crystals were also obtained. Scanning pulsed-electron microscopy with the acquired spatiotemporal resolutions, and its efficient heat-dissipation feature, is now poised to provide in situ 4D imaging and with environmental capability. PMID:20696933

Dissipative gravitational bouncer on a vibrating surface

NASA Astrophysics Data System (ADS)

Espinoza Ortiz, J. S.; Lagos, R. E.

2017-12-01

We study the dynamical behavior of a particle flying under the influence of a gravitational field, with dissipation constant λ (Stokes-like), colliding successive times against a rigid surface vibrating harmonically with restitution coefficient α. We define re-scaled dimensionless dynamical variables, such as the relative particle velocity Ω with respect to the surface’s velocity; and the real parameter τ accounting for the temporal evolution of the system. At the particle-surface contact point and for the k‧th collision, we construct the mapping described by (τk ; Ω k ) in order to analyze the system’s nonlinear dynamical behavior. From the dynamical mapping, the fixed point trajectory is computed and its stability is analyzed. We find the dynamical behavior of the fixed point trajectory to be stable or unstable, depending on the values of the re-scaled vibrating surface amplitude Γ, the restitution coefficient α and the damping constant λ. Other important dynamical aspects such as the phase space volume and the one cycle vibrating surface (decomposed into absorbing and transmitting regions) are also discussed. Furthermore, the model rescues well known results in the limit λ = 0.

Ultrafast photophysics of transition metal complexes.

PubMed

Chergui, Majed

2015-03-17

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

Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses.

PubMed

Calegari, F; Ayuso, D; Trabattoni, A; Belshaw, L; De Camillis, S; Anumula, S; Frassetto, F; Poletto, L; Palacios, A; Decleva, P; Greenwood, J B; Martín, F; Nisoli, M

2014-10-17

In the past decade, attosecond technology has opened up the investigation of ultrafast electronic processes in atoms, simple molecules, and solids. Here, we report the application of isolated attosecond pulses to prompt ionization of the amino acid phenylalanine and the subsequent detection of ultrafast dynamics on a sub-4.5-femtosecond temporal scale, which is shorter than the vibrational response of the molecule. The ability to initiate and observe such electronic dynamics in polyatomic molecules represents a crucial step forward in attosecond science, which is progressively moving toward the investigation of more and more complex systems. Copyright © 2014, American Association for the Advancement of Science.

Ultrafast optical measurements of surface waves on a patterned layered nanostructure

NASA Astrophysics Data System (ADS)

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

2015-03-01

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

Surface separation investigation of ultrafast pulsed laser welding

NASA Astrophysics Data System (ADS)

Chen, Jianyong; Carter, Richard M.; Thomson, Robert R.; Hand, Duncan P.

2016-03-01

Techniques for joining materials, especially optical materials such as glass to structural materials such as metals, or to other optical materials, while maintaining their surface and optical properties are essential for a wide range of industrial applications. Adhesive bonding is commonly used but leads to many issues including optical surface contamination and outgassing. It is possible to generate welds using an ultra-short pulsed laser process, whereby two flat material surfaces are brought into close contact and the laser is focused through the optical material onto the interface. Highly localised melting and rapid resolidification form a strong bond between the two surfaces whilst avoiding significant heating of the surrounding material, which is important for joining materials with different thermal expansion coefficients. Previous reports on ultrafast laser welding have identified a requirement for the surface separation gap to be less than 500nm in order to avoid cracking or ablation at the interface. We have investigated techniques for increasing this gap (to reduce weld fit-up problems), and tested by bonding two surfaces with a weld-controlled gap. These gaps were generated either by a series of etched grooves on the surface of one of the substrates, or by using a cylindrical lens as a substrate. By careful optimisation of parameters such as laser power, process speed and focal position, we were able to demonstrate successful welding with a gap of up to 3μm.

Mixed quantum-classical simulations of the vibrational relaxation of photolyzed carbon monoxide in a hemoprotein

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

Schubert, Alexander, E-mail: schubert@irsamc.ups-tlse.fr; Meier, Christoph; Falvo, Cyril

2016-08-07

We present mixed quantum-classical simulations on relaxation and dephasing of vibrationally excited carbon monoxide within a protein environment. The methodology is based on a vibrational surface hopping approach treating the vibrational states of CO quantum mechanically, while all remaining degrees of freedom are described by means of classical molecular dynamics. The CO vibrational states form the “surfaces” for the classical trajectories of protein and solvent atoms. In return, environmentally induced non-adiabatic couplings between these states cause transitions describing the vibrational relaxation from first principles. The molecular dynamics simulation yields a detailed atomistic picture of the energy relaxation pathways, taking themore » molecular structure and dynamics of the protein and its solvent fully into account. Using the ultrafast photolysis of CO in the hemoprotein FixL as an example, we study the relaxation of vibrationally excited CO and evaluate the role of each of the FixL residues forming the heme pocket.« less

Ultrafast inter- and intramolecular vibrational energy transfer between molecules at interfaces studied by time- and polarization-resolved SFG spectroscopy.

PubMed

Yamamoto, Susumu; Ghosh, Avishek; Nienhuys, Han-Kwang; Bonn, Mischa

2010-10-28

We present experimental results on femtosecond time-resolved surface vibrational spectroscopy aimed at elucidating the sub-picosecond reorientational dynamics of surface molecules. The approach, which relies on polarization- and time-resolved surface sum frequency generation (SFG), provides a general means to monitor interfacial reorientational dynamics through vibrations inherent in surface molecules in their electronic ground state. The technique requires an anisotropic vibrational excitation of surface molecules using orthogonally polarized infrared excitation light. The decay of the resulting anisotropy is followed in real-time. We employ the technique to reveal the reorientational dynamics of vibrational transition dipoles of long-chain primary alcohols on the water surface, and of water molecules at the water-air interface. The results demonstrate that, in addition to reorientational motion of specific molecules or molecular groups at the interface, inter- and intramolecular energy transfer processes can serve to scramble the initial anisotropy very efficiently. In the two exemplary cases demonstrated here, energy transfer occurs much faster than reorientational motion of interfacial molecules. This has important implications for the interpretation of static SFG spectra. Finally, we suggest experimental schemes and strategies to decouple effects resulting from energy transfer from those associated with surface molecular motion.

Origin of Vibrational Spectroscopic Response at Ice Surface.

PubMed

Ishiyama, Tatsuya; Takahashi, Hideaki; Morita, Akihiro

2012-10-18

Since the basal plane surface of ice was first observed by sum frequency generation, an extraordinarily intense band for the hydrogen(H)-bonded OH stretching vibration has been a matter of debate. We elucidate the remarkable spectral feature of the ice surface by quantum mechanics/molecular mechanics calculations. The intense H-bonded band is originated mostly from the "bilayer-stitching" modes of a few surface bilayers, through significant intermolecular charge transfer. The mechanism of enhanced signal is sensitive to the order of the tetrahedral ice structure, as the charge transfer is coupled to the vibrational delocalization.

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.

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.

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.

Vibrational energy flow in photoactive yellow protein revealed by infrared pump-visible probe spectroscopy.

PubMed

Nakamura, Ryosuke; Hamada, Norio

2015-05-14

Vibrational energy flow in the electronic ground state of photoactive yellow protein (PYP) is studied by ultrafast infrared (IR) pump-visible probe spectroscopy. Vibrational modes of the chromophore and the surrounding protein are excited with a femtosecond IR pump pulse, and the subsequent vibrational dynamics in the chromophore are selectively probed with a visible probe pulse through changes in the absorption spectrum of the chromophore. We thus obtain the vibrational energy flow with four characteristic time constants. The vibrational excitation with an IR pulse at 1340, 1420, 1500, or 1670 cm(-1) results in ultrafast intramolecular vibrational redistribution (IVR) with a time constant of 0.2 ps. The vibrational modes excited through the IVR process relax to the initial ground state with a time constant of 6-8 ps in parallel with vibrational cooling with a time constant of 14 ps. In addition, upon excitation with an IR pulse at 1670 cm(-1), we observe the energy flow from the protein backbone to the chromophore that occurs with a time constant of 4.2 ps.

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.

Ultrafast dynamics of ligand and substrate interaction in endothelial nitric oxide synthase under Soret excitation.

PubMed

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

2016-01-01

Ultrafast transient absorption spectroscopy of endothelial NOS oxygenase domain (eNOS-oxy) was performed to study dynamics of ligand or substrate interaction under Soret band excitation. Photo-excitation dissociates imidazole ligand in <300fs, then followed by vibrational cooling and recombination within 2ps. Such impulsive bond breaking and late rebinding generate proteinquakes, which relaxes in several tens of picoseconds. The photo excited dynamics of eNOS-oxy with L-arginine substrate mainly occurs at the local site of heme, including ultrafast internal conversion within 400fs, vibrational cooling, charge transfer, and complete ground-state recovery within 1.4ps. The eNOS-oxy without additive is partially bound with water molecule, thus its photoexcited dynamics also shows ligand dissociation in <800fs. Then it followed by vibrational cooling coupled with charge transfer in 4.8ps, and recombination of ligand to distal side of heme in 12ps. Copyright © 2016 Elsevier B.V. All rights reserved.

Observation of the adsorption and desorption of vibrationally excited molecules on a metal surface

NASA Astrophysics Data System (ADS)

Shirhatti, Pranav R.; Rahinov, Igor; Golibrzuch, Kai; Werdecker, Jörn; Geweke, Jan; Altschäffel, Jan; Kumar, Sumit; Auerbach, Daniel J.; Bartels, Christof; Wodtke, Alec M.

2018-06-01

The most common mechanism of catalytic surface chemistry is that of Langmuir and Hinshelwood (LH). In the LH mechanism, reactants adsorb, become thermalized with the surface, and subsequently react. The measured vibrational (relaxation) lifetimes of molecules adsorbed at metal surfaces are in the range of a few picoseconds. As a consequence, vibrational promotion of LH chemistry is rarely observed, with the exception of LH reactions occurring via a molecular physisorbed intermediate. Here, we directly detect adsorption and subsequent desorption of vibrationally excited CO molecules from a Au(111) surface. Our results show that CO (v = 1) survives on a Au(111) surface for 1 × 10-10 s. Such long vibrational lifetimes for adsorbates on metal surfaces are unexpected and pose an interesting challenge to the current understanding of vibrational energy dissipation on metal surfaces. They also suggest that vibrational promotion of surface chemistry might be more common than is generally believed.

Vibrational cross-angles in condensed molecules: a structural tool.

PubMed

Chen, Hailong; Zhang, Yufan; Li, Jiebo; Liu, Hongjun; Jiang, De-En; Zheng, Junrong

2013-09-05

The fluctuations of three-dimensional molecular conformations of a molecule in different environments play critical roles in many important chemical and biological processes. X-ray diffraction (XRD) techniques and nuclear magnetic resonance (NMR) methods are routinely applied to monitor the molecular conformations in condensed phases. However, some special requirements of the methods have prevented them from exploring many molecular phenomena at the current stage. Here, we introduce another method to resolve molecular conformations based on an ultrafast MIR/T-Hz multiple-dimensional vibrational spectroscopic technique. The model molecule (4'-methyl-2'-nitroacetanilide, MNA) is prepared in two of its crystalline forms and liquid samples. Two polarized ultrafast infrared pulses are then used to determine the cross-angles of vibrational transition moment directions by exciting one vibrational band and detecting the induced response on another vibrational band of the molecule. The vibrational cross-angles are then converted into molecular conformations with the aid of calculations. The molecular conformations determined by the method are supported by X-ray diffraction and molecular dynamics simulation results. The experimental results suggest that thermodynamic interactions with solvent molecules are not altering the molecular conformations of MNA in the solutions to control their ultimate conformations in the crystals.

Vibration Influences Haptic Perception of Surface Compliance During Walking

PubMed Central

Visell, Yon; Giordano, Bruno L.; Millet, Guillaume; Cooperstock, Jeremy R.

2011-01-01

Background The haptic perception of ground compliance is used for stable regulation of dynamic posture and the control of locomotion in diverse natural environments. Although rarely investigated in relation to walking, vibrotactile sensory channels are known to be active in the discrimination of material properties of objects and surfaces through touch. This study investigated how the perception of ground surface compliance is altered by plantar vibration feedback. Methodology/Principal Findings Subjects walked in shoes over a rigid floor plate that provided plantar vibration feedback, and responded indicating how compliant it felt, either in subjective magnitude or via pairwise comparisons. In one experiment, the compliance of the floor plate was also varied. Results showed that perceived compliance of the plate increased monotonically with vibration feedback intensity, and depended to a lesser extent on the temporal or frequency distribution of the feedback. When both plate stiffness (inverse compliance) and vibration amplitude were manipulated, the effect persisted, with both factors contributing to compliance perception. A significant influence of vibration was observed even for amplitudes close to psychophysical detection thresholds. Conclusions/Significance These findings reveal that vibrotactile sensory channels are highly salient to the perception of surface compliance, and suggest that correlations between vibrotactile sensory information and motor activity may be of broader significance for the control of human locomotion than has been previously acknowledged. PMID:21464979

Surface hopping simulation of vibrational predissociation of methanol dimer

NASA Astrophysics Data System (ADS)

Jiang, Ruomu; Sibert, Edwin L.

2012-06-01

The mixed quantum-classical surface hopping method is applied to the vibrational predissociation of methanol dimer, and the results are compared to more exact quantum calculations. Utilizing the vibrational SCF basis, the predissociation problem is cast into a curve crossing problem between dissociative and quasibound surfaces with different vibrational character. The varied features of the dissociative surfaces, arising from the large amplitude OH torsion, generate rich predissociation dynamics. The fewest switches surface hopping algorithm of Tully [J. Chem. Phys. 93, 1061 (1990), 10.1063/1.459170] is applied to both diabatic and adiabatic representations. The comparison affords new insight into the criterion for selecting the suitable representation. The adiabatic method's difficulty with low energy trajectories is highlighted. In the normal crossing case, the diabatic calculations yield good results, albeit showing its limitation in situations where tunneling is important. The quadratic scaling of the rates on coupling strength is confirmed. An interesting resonance behavior is identified and is dealt with using a simple decoherence scheme. For low lying dissociative surfaces that do not cross the quasibound surface, the diabatic method tends to overestimate the predissociation rate whereas the adiabatic method is qualitatively correct. Analysis reveals the major culprits involve Rabi-like oscillation, treatment of classically forbidden hops, and overcoherence. Improvements of the surface hopping results are achieved by adopting a few changes to the original surface hopping algorithms.

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.

Graphene-clad microfibre saturable absorber for ultrafast fibre lasers.

PubMed

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

2016-05-16

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

Graphene-clad microfibre saturable absorber for ultrafast fibre lasers

PubMed Central

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

2016-01-01

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

New vibration-assisted magnetic abrasive polishing (VAMAP) method for microstructured surface finishing.

PubMed

Guo, Jiang; Kum, Chun Wai; Au, Ka Hing; Tan, Zhi'En Eddie; Wu, Hu; Liu, Kui

2016-06-13

In order to polish microstructured surface without deteriorating its profile, we propose a new vibration-assisted magnetic abrasive polishing (VAMAP) method. In this method, magnetic force guarantees that the magnetic abrasives can well contact the microstructured surface and access the corners of microstructures while vibration produces a relative movement between microstructures and magnetic abrasives. As the vibration direction is parallel to the microstructures, the profile of the microstructures will not be deteriorated. The relation between vibration and magnetic force was analyzed and the feasibility of this method was experimentally verified. The results show that after polishing, the surface finish around microstructures was significantly improved while the profile of microstructures was well maintained.

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.

Femtosecond nonlinear ultrasonics in gold probed with ultrashort surface plasmons.

PubMed

Temnov, Vasily V; Klieber, Christoph; Nelson, Keith A; Thomay, Tim; Knittel, Vanessa; Leitenstorfer, Alfred; Makarov, Denys; Albrecht, Manfred; Bratschitsch, Rudolf

2013-01-01

Fundamental interactions induced by lattice vibrations on ultrafast time scales have become increasingly important for modern nanoscience and technology. Experimental access to the physical properties of acoustic phonons in the terahertz-frequency range and over the entire Brillouin zone is crucial for understanding electric and thermal transport in solids and their compounds. Here we report on the generation and nonlinear propagation of giant (1 per cent) acoustic strain pulses in hybrid gold/cobalt bilayer structures probed with ultrafast surface plasmon interferometry. This new technique allows for unambiguous characterization of arbitrary ultrafast acoustic transients. The giant acoustic pulses experience substantial nonlinear reshaping after a propagation distance of only 100 nm in a crystalline gold layer. Excellent agreement with the Korteveg-de Vries model points to future quantitative nonlinear femtosecond terahertz-ultrasonics at the nano-scale in metals at room temperature.

Surface vibrational modes in disk-shaped resonators.

PubMed

Dmitriev, A V; Gritsenko, D S; Mitrofanov, V P

2014-03-01

The natural frequencies and distributions of displacement components for the surface vibrational modes in thin isotropic elastic disks are calculated. In particular, the research is focused on even solutions for low-lying resonant vibrations with large angular wave numbers. Several families of modes are found which are interpreted as modified surface modes of an infinitely long cylinder and Lamb modes of a plate. The results of calculation are compared with the results of the experimental measurements of vibrational modes generated by means of resonant excitation in duraluminum disk with radius of ≈90 mm and thickness of 16 mm in the frequency range of 130-200 kHz. An excellent agreement between the calculated and measured frequencies is found. Measurements of the structure of the resonant peaks show splitting of some modes. About a half of the measured modes has splitting Δfsplit/fmode at the level of the order of 10(-5). The Q-factors of all modes measured in vacuum lie in the interval (2…3)×10(5). This value is typical for duraluminum mechanical resonators in the ultrasonic frequency range. Copyright © 2013 Elsevier B.V. All rights reserved.

Expansion Hamiltonian model for a diatomic molecule adsorbed on a surface: Vibrational states of the CO/Cu(100) system including surface vibrations

NASA Astrophysics Data System (ADS)

Meng, Qingyong; Meyer, Hans-Dieter

2015-10-01

Molecular-surface studies are often done by assuming a corrugated, static (i.e., rigid) surface. To be able to investigate the effects that vibrations of surface atoms may have on spectra and cross sections, an expansion Hamiltonian model is proposed on the basis of the recently reported [R. Marquardt et al., J. Chem. Phys. 132, 074108 (2010)] SAP potential energy surface (PES), which was built for the CO/Cu(100) system with a rigid surface. In contrast to other molecule-surface coupling models, such as the modified surface oscillator model, the coupling between the adsorbed molecule and the surface atoms is already included in the present expansion SAP-PES model, in which a Taylor expansion around the equilibrium positions of the surface atoms is performed. To test the quality of the Taylor expansion, a direct model, that is avoiding the expansion, is also studied. The latter, however, requests that there is only one movable surface atom included. On the basis of the present expansion and direct models, the effects of a moving top copper atom (the one to which CO is bound) on the energy levels of a bound CO/Cu(100) system are studied. For this purpose, the multiconfiguration time-dependent Hartree calculations are carried out to obtain the vibrational fundamentals and overtones of the CO/Cu(100) system including a movable top copper atom. In order to interpret the results, a simple model consisting of two coupled harmonic oscillators is introduced. From these calculations, the vibrational levels of the CO/Cu(100) system as function of the frequency of the top copper atom are discussed.

Expansion Hamiltonian model for a diatomic molecule adsorbed on a surface: Vibrational states of the CO/Cu(100) system including surface vibrations

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

Meng, Qingyong, E-mail: mengqingyong@dicp.ac.cn; Meyer, Hans-Dieter, E-mail: hans-dieter.meyer@pci.uni-heidelberg.de

2015-10-28

Molecular-surface studies are often done by assuming a corrugated, static (i.e., rigid) surface. To be able to investigate the effects that vibrations of surface atoms may have on spectra and cross sections, an expansion Hamiltonian model is proposed on the basis of the recently reported [R. Marquardt et al., J. Chem. Phys. 132, 074108 (2010)] SAP potential energy surface (PES), which was built for the CO/Cu(100) system with a rigid surface. In contrast to other molecule-surface coupling models, such as the modified surface oscillator model, the coupling between the adsorbed molecule and the surface atoms is already included in themore » present expansion SAP-PES model, in which a Taylor expansion around the equilibrium positions of the surface atoms is performed. To test the quality of the Taylor expansion, a direct model, that is avoiding the expansion, is also studied. The latter, however, requests that there is only one movable surface atom included. On the basis of the present expansion and direct models, the effects of a moving top copper atom (the one to which CO is bound) on the energy levels of a bound CO/Cu(100) system are studied. For this purpose, the multiconfiguration time-dependent Hartree calculations are carried out to obtain the vibrational fundamentals and overtones of the CO/Cu(100) system including a movable top copper atom. In order to interpret the results, a simple model consisting of two coupled harmonic oscillators is introduced. From these calculations, the vibrational levels of the CO/Cu(100) system as function of the frequency of the top copper atom are discussed.« less

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.

Normal-mode selectivity in ultrafast Raman excitations in C60

NASA Astrophysics Data System (ADS)

Zhang, G. P.; George, Thomas F.

2006-01-01

Ultrafast Raman spectra are a powerful tool to probe vibrational excitations, but inherently they are not normal-mode specific. For a system as complicated as C60 , there is no general rule to target a specific mode. A detailed study presented here aims to investigate normal-mode selectivity in C60 by an ultrafast laser. To accurately measure mode excitation, we formally introduce the kinetic-energy-based normal-mode analysis which overcomes the difficulty with the strong lattice anharmonicity and relaxation. We first investigate the resonant excitation and find that mode selectivity is normally difficult to achieve. However, for off-resonant excitations, it is possible to selectively excite a few modes in C60 by properly choosing an optimal laser pulse duration, which agrees with previous experimental and theoretical findings. Going beyond the phenomenological explanation, our study shines new light on the origin of the optimal duration: The phase matching between the laser field and mode vibration determines which mode is strongly excited or suppressed. This finding is very robust and should be a useful guide for future experimental and theoretical studies in more complicated systems.

Normal mode selectivity in ultrafast Raman excitations in C60

NASA Astrophysics Data System (ADS)

Zhang, Guoping; George, Thomas F.

2006-05-01

Ultrafast Raman spectra are a powerful tool to probe vibrational excitations, but inherently they are not normal-mode specific. For a system as complicated as C60, there is no general rule to target a specific mode. A detailed study presented here aims to investigate normal mode selectivity in C60 by an ultrafast laser. To accurately measure mode excitation, we formally introduce the kinetic energy-based normal mode analysis which overcomes the difficulty with the strong lattice anharmonicity and relaxation. We first investigate the resonant excitation and find that mode selectivity is normally difficult to achieve. However, for off-resonant excitations, it is possible to selectively excite a few modes in C60 by properly choosing an optimal laser pulse duration, which agrees with previous experimental and theoretical findings. Going beyond the phenomenological explanation, our study shines new light on the origin of the optimal duration: The phase matching between laser field and mode vibration determines which mode is strongly excited or suppressed. This finding is very robust and may be a useful guide for future experimental and theoretical studies in more complicated systems.

Ultrafast vibrational energy flow in water monomers in acetonitrile

NASA Astrophysics Data System (ADS)

Dahms, Fabian; Costard, Rene; Nibbering, Erik T. J.; Elsaesser, Thomas

2016-05-01

Vibrational relaxation of the OH stretching and bending modes of water monomers in acetonitrile is studied by two-color pump-probe experiments in a frequency range from 1400 to 3800 cm-1. Measurements with resonant infrared excitation reveal vibrational lifetimes of 6.4 ± 1.0 ps of the OH stretching modes and 4.0 ± 0.5 ps of the OH bending mode. After OH stretching excitation, the OH bending mode shows an instantaneous response, a hallmark of the anharmonic coupling of stretching and bending modes, and a delayed population buildup by relaxation of the stretching via the bending mode. The relaxation steps are discussed within the framework of current theoretical pictures of water's vibrational relaxation.

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

Real-Space Imaging of Carrier Dynamics of Materials Surfaces by Second-Generation Four-Dimensional Scanning Ultrafast Electron Microscopy.

PubMed

Sun, Jingya; Melnikov, Vasily A; Khan, Jafar I; Mohammed, Omar F

2015-10-01

In the fields of photocatalysis and photovoltaics, ultrafast dynamical processes, including carrier trapping and recombination on material surfaces, are among the key factors that determine the overall energy conversion efficiency. A precise knowledge of these dynamical events on the nanometer (nm) and femtosecond (fs) scales was not accessible until recently. The only way to access such fundamental processes fully is to map the surface dynamics selectively in real space and time. In this study, we establish a second generation of four-dimensional scanning ultrafast electron microscopy (4D S-UEM) and demonstrate the ability to record time-resolved images (snapshots) of material surfaces with 650 fs and ∼5 nm temporal and spatial resolutions, respectively. In this method, the surface of a specimen is excited by a clocking optical pulse and imaged using a pulsed primary electron beam as a probe pulse, generating secondary electrons (SEs), which are emitted from the surface of the specimen in a manner that is sensitive to the local electron/hole density. This method provides direct and controllable information regarding surface dynamics. We clearly demonstrate how the surface morphology, grains, defects, and nanostructured features can significantly impact the overall dynamical processes on the surface of photoactive-materials. In addition, the ability to access two regimes of dynamical probing in a single experiment and the energy loss of SEs in semiconductor-nanoscale materials will also be discussed.

Vibronic coupling explains the ultrafast carotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

NASA Astrophysics Data System (ADS)

Perlík, Václav; Seibt, Joachim; Cranston, Laura J.; Cogdell, Richard J.; Lincoln, Craig N.; Savolainen, Janne; Šanda, František; Mančal, Tomáš; Hauer, Jürgen

2015-06-01

The initial energy transfer steps in photosynthesis occur on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that Förster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which lead to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited states as part of the system's Hamiltonian, reproduces all measured quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels on the carotenoid electronic ground state play the central role in the excited state population transfer to bacteriochlorophyll; resonance between the donor-acceptor energy gap and the vibrational ground state energies is the physical basis of the ultrafast energy transfer rates in these systems.

Localized surface plasmons in vibrating graphene nanodisks

NASA Astrophysics Data System (ADS)

Wang, Weihua; Li, Bo-Hong; Stassen, Erik; Mortensen, N. Asger; Christensen, Johan

2016-02-01

Localized surface plasmons are confined collective oscillations of electrons in metallic nanoparticles. When driven by light, the optical response is dictated by geometrical parameters and the dielectric environment and plasmons are therefore extremely important for sensing applications. Plasmons in graphene disks have the additional benefit of being highly tunable via electrical stimulation. Mechanical vibrations create structural deformations in ways where the excitation of localized surface plasmons can be strongly modulated. We show that the spectral shift in such a scenario is determined by a complex interplay between the symmetry and shape of the modal vibrations and the plasmonic mode pattern. Tuning confined modes of light in graphene via acoustic excitations, paves new avenues in shaping the sensitivity of plasmonic detectors, and in the enhancement of the interaction with optical emitters, such as molecules, for future nanophotonic devices.

Surface vibrational structure at alkane liquid/vapor interfaces

NASA Astrophysics Data System (ADS)

Esenturk, Okan; Walker, Robert A.

2006-11-01

Broadband vibrational sum frequency spectroscopy (VSFS) has been used to examine the surface structure of alkane liquid/vapor interfaces. The alkanes range in length from n-nonane (C9H20) to n-heptadecane (C17H36), and all liquids except heptadecane are studied at temperatures well above their bulk (and surface) freezing temperatures. Intensities of vibrational bands in the CH stretching region acquired under different polarization conditions show systematic, chain length dependent changes. Data provide clear evidence of methyl group segregation at the liquid/vapor interface, but two different models of alkane chain structure can predict chain length dependent changes in band intensities. Each model leads to a different interpretation of the extent to which different chain segments contribute to the anisotropic interfacial region. One model postulates that changes in vibrational band intensities arise solely from a reduced surface coverage of methyl groups as alkane chain length increases. The additional methylene groups at the surface must be randomly distributed and make no net contribution to the observed VSF spectra. The second model considers a simple statistical distribution of methyl and methylene groups populating a three dimensional, interfacial lattice. This statistical picture implies that the VSF signal arises from a region extending several functional groups into the bulk liquid, and that the growing fraction of methylene groups in longer chain alkanes bears responsibility for the observed spectral changes. The data and resulting interpretations provide clear benchmarks for emerging theories of molecular structure and organization at liquid surfaces, especially for liquids lacking strong polar ordering.

Probing the Ultrafast Energy Dissipation Mechanism of the Sunscreen Oxybenzone after UVA Irradiation.

PubMed

Baker, Lewis A; Horbury, Michael D; Greenough, Simon E; Coulter, Philip M; Karsili, Tolga N V; Roberts, Gareth M; Orr-Ewing, Andrew J; Ashfold, Michael N R; Stavros, Vasilios G

2015-04-16

Oxybenzone is a common constituent of many commercially available sunscreens providing photoprotection from ultraviolet light incident on the skin. Femtosecond transient electronic and vibrational absorption spectroscopies have been used to investigate the nonradiative relaxation pathways of oxybenzone in cyclohexane and methanol after excitation in the UVA region. The present data suggest that the photoprotective properties of oxybenzone can be understood in terms of an initial ultrafast excited state enol → keto tautomerization, followed by efficient internal conversion and subsequent vibrational relaxation to the ground state (enol) tautomer.

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.

Multidimensional infrared spectroscopy reveals the vibrational and solvation dynamics of isoniazid

NASA Astrophysics Data System (ADS)

Shaw, Daniel J.; Adamczyk, Katrin; Frederix, Pim W. J. M.; Simpson, Niall; Robb, Kirsty; Greetham, Gregory M.; Towrie, Michael; Parker, Anthony W.; Hoskisson, Paul A.; Hunt, Neil T.

2015-06-01

The results of infrared spectroscopic investigations into the band assignments, vibrational relaxation, and solvation dynamics of the common anti-tuberculosis treatment Isoniazid (INH) are reported. INH is known to inhibit InhA, a 2-trans-enoyl-acyl carrier protein reductase enzyme responsible for the maintenance of cell walls in Mycobacterium tuberculosis but as new drug-resistant strains of the bacterium appear, next-generation therapeutics will be essential to combat the rise of the disease. Small molecules such as INH offer the potential for use as a biomolecular marker through which ultrafast multidimensional spectroscopies can probe drug binding and so inform design strategies but a complete characterization of the spectroscopy and dynamics of INH in solution is required to inform such activity. Infrared absorption spectroscopy, in combination with density functional theory calculations, is used to assign the vibrational modes of INH in the 1400-1700 cm-1 region of the infrared spectrum while ultrafast multidimensional spectroscopy measurements determine the vibrational relaxation dynamics and the effects of solvation via spectral diffusion of the carbonyl stretching vibrational mode. These results are discussed in the context of previous linear spectroscopy studies on solid-phase INH and its usefulness as a biomolecular probe.

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.

Predicting surface vibration from underground railways through inhomogeneous soil

NASA Astrophysics Data System (ADS)

Jones, Simon; Hunt, Hugh

2012-04-01

Noise and vibration from underground railways is a major source of disturbance to inhabitants near subways. To help designers meet noise and vibration limits, numerical models are used to understand vibration propagation from these underground railways. However, the models commonly assume the ground is homogeneous and neglect to include local variability in the soil properties. Such simplifying assumptions add a level of uncertainty to the predictions which is not well understood. The goal of the current paper is to quantify the effect of soil inhomogeneity on surface vibration. The thin-layer method (TLM) is suggested as an efficient and accurate means of simulating vibration from underground railways in arbitrarily layered half-spaces. Stochastic variability of the soil's elastic modulus is introduced using a K-L expansion; the modulus is assumed to have a log-normal distribution and a modified exponential covariance kernel. The effect of horizontal soil variability is investigated by comparing the stochastic results for soils varied only in the vertical direction to soils with 2D variability. Results suggest that local soil inhomogeneity can significantly affect surface velocity predictions; 90 percent confidence intervals showing 8 dB averages and peak values up to 12 dB are computed. This is a significant source of uncertainty and should be considered when using predictions from models assuming homogeneous soil properties. Furthermore, the effect of horizontal variability of the elastic modulus on the confidence interval appears to be negligible. This suggests that only vertical variation needs to be taken into account when modelling ground vibration from underground railways.

Recent advances in multidimensional ultrafast spectroscopy

NASA Astrophysics Data System (ADS)

Oliver, Thomas A. A.

2018-01-01

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

Recent advances in multidimensional ultrafast spectroscopy

PubMed Central

2018-01-01

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

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.

Ultrafast electronic and vibrational dynamics of stabilized A state mutants of the green fluorescent protein (GFP): Snipping the proton wire

NASA Astrophysics Data System (ADS)

Stoner-Ma, Deborah; Jaye, Andrew A.; Ronayne, Kate L.; Nappa, Jérôme; Tonge, Peter J.; Meech, Stephen R.

2008-06-01

Two blue absorbing and emitting mutants (S65G/T203V/E222Q and S65T at pH 5.5) of the green fluorescent protein (GFP) have been investigated through ultrafast time resolved infra-red (TRIR) and fluorescence spectroscopy. In these mutants, in which the excited state proton transfer reaction observed in wild-type GFP has been blocked, the photophysics are dominated by the neutral A state. It was found that the A∗ excited state lifetime is short, indicating that it is relatively less stabilised in the protein matrix than the anionic form. However, the lifetime of the A state can be increased through modifications to the protein structure. The TRIR spectra show that a large shifts in protein vibrational modes on excitation of the A state occurs in both these GFP mutants. This is ascribed to a change in H-bonding interactions between the protein matrix and the excited state.

Fast and ultrafast endocytosis.

PubMed

Watanabe, Shigeki; Boucrot, Emmanuel

2017-08-01

Clathrin-mediated endocytosis (CME) is the main endocytic pathway supporting housekeeping functions in cells. However, CME may be too slow to internalize proteins from the cell surface during certain physiological processes such as reaction to stress hormones ('fight-or-flight' reaction), chemotaxis or compensatory endocytosis following exocytosis of synaptic vesicles or hormone-containing vesicles. These processes take place on a millisecond to second timescale and thus require very rapid cellular reaction to prevent overstimulation or exhaustion of the response. There are several fast endocytic processes identified so far: macropinocytosis, activity-dependent bulk endocytosis (ABDE), fast-endophilin-mediated endocytosis (FEME), kiss-and-run and ultrafast endocytosis. All are clathrin-independent and are not constitutively active but may use different molecular mechanisms to rapidly remove receptors and proteins from the cell surface. Here, we review our current understanding of fast and ultrafast endocytosis, their functions, and molecular mechanisms. Copyright © 2017 Elsevier Ltd. All rights reserved.

Understanding of the Formation of Micro/Nanoscale Structures on Metal Surfaces by Ultrafast Pulse Laser Processing

NASA Astrophysics Data System (ADS)

Peng, Edwin

In the recent decades, there has been much interest in functionalized surfaces produced by ultrafast laser processing. Using pulse lasers with nanosecond to femtosecond time scale, a wide range of micro/nanoscale structures can be produced on virtually all metal surfaces. These surface structures create special optoelectronic, wetting, and tribological properties with a diverse range of potential applications. The formation mechanisms of these surface structures, especially microscale, mound-like structures, are not fully understood. There has been wide study of ultrafast laser processing of metals. Yet, the proposed formation models present in current literature often lack sufficient experimental verification. Specifically, many studies are limited to surface characterization, e.g. scanning electron microscopy of the surfaces of these micro/nanoscale structures. Valuable insight into the physical processes responsible for formation can be obtained if standard material science characterization methods are performed across the entire mound. In our study, we examined mound-like structures formed on three metal alloys. Using cross section and 3D slice and view operations by a dual beam scanning electron microscope-focused ion beam, the interior microstructures of these mounds are revealed. Taking advantage of amorphous phase formation during laser processing of Ni60Nb40, we verified the fluence-dependent formation model: mounds formed at low fluence are primarily the result of ablation while mounds formed at high fluence are formed by both ablation and rapid resolidification by hydrodynamical fluid flow. For the first time, we revealed the cross section of a wide variety of mound-like structures on titanium surfaces. The increased contribution to mound formation by fluid flow with increasing fluence was observed. Finally, a 3D scanning electron microscopy technique was applied for mounds produced on silver surface by delayed-pulse laser processing. The interior

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.

Coherent Amplification of Ultrafast Molecular Dynamics in an Optical Oscillator

NASA Astrophysics Data System (ADS)

Aharonovich, Igal; Pe'er, Avi

2016-02-01

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

Passive Optical Technique to Measure Physical Properties of a Vibrating Surface

DTIC Science & Technology

2014-01-01

it is not necessary to understand the details of a non-Lambertian BRDF to detect surface vibration phenomena, an accurate model incorporating physics...summarize the discussion of BRDF , while a physics-based BRDF model is not necessary to use scattered light as a surface vibration diagnostic, it may...penalty for failing to comply with a collection of information if it does not display a currently valid OMB control number. 1. REPORT DATE 2014 2

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.

Terahertz Emission from Hybrid Perovskites Driven by Ultrafast Charge Separation and Strong Electron-Phonon Coupling.

PubMed

Guzelturk, Burak; Belisle, Rebecca A; Smith, Matthew D; Bruening, Karsten; Prasanna, Rohit; Yuan, Yakun; Gopalan, Venkatraman; Tassone, Christopher J; Karunadasa, Hemamala I; McGehee, Michael D; Lindenberg, Aaron M

2018-03-01

Unusual photophysical properties of organic-inorganic hybrid perovskites have not only enabled exceptional performance in optoelectronic devices, but also led to debates on the nature of charge carriers in these materials. This study makes the first observation of intense terahertz (THz) emission from the hybrid perovskite methylammonium lead iodide (CH 3 NH 3 PbI 3 ) following photoexcitation, enabling an ultrafast probe of charge separation, hot-carrier transport, and carrier-lattice coupling under 1-sun-equivalent illumination conditions. Using this approach, the initial charge separation/transport in the hybrid perovskites is shown to be driven by diffusion and not by surface fields or intrinsic ferroelectricity. Diffusivities of the hot and band-edge carriers along the surface normal direction are calculated by analyzing the emitted THz transients, with direct implications for hot-carrier device applications. Furthermore, photogenerated carriers are found to drive coherent terahertz-frequency lattice distortions, associated with reorganizations of the lead-iodide octahedra as well as coupled vibrations of the organic and inorganic sublattices. This strong and coherent carrier-lattice coupling is resolved on femtosecond timescales and found to be important both for resonant and far-above-gap photoexcitation. This study indicates that ultrafast lattice distortions play a key role in the initial processes associated with charge transport. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Terahertz Emission from Hybrid Perovskites Driven by Ultrafast Charge Separation and Strong Electron-Phonon Coupling

DOE PAGES

Guzelturk, Burak; Belisle, Rebecca A.; Smith, Matthew D.; ...

2018-01-23

Unusual photophysical properties of organic–inorganic hybrid perovskites have not only enabled exceptional performance in optoelectronic devices, but also led to debates on the nature of charge carriers in these materials. This study makes the first observation of intense terahertz (THz) emission from the hybrid perovskite methylammonium lead iodide (CH 3NH 3PbI 3) following photoexcitation, enabling an ultrafast probe of charge separation, hot–carrier transport, and carrier–lattice coupling under 1–sun–equivalent illumination conditions. Using this approach, the initial charge separation/transport in the hybrid perovskites is shown to be driven by diffusion and not by surface fields or intrinsic ferroelectricity. Diffusivities of the hotmore » and band–edge carriers along the surface normal direction are calculated by analyzing the emitted THz transients, with direct implications for hot–carrier device applications. Furthermore, photogenerated carriers are found to drive coherent terahertz–frequency lattice distortions, associated with reorganizations of the lead–iodide octahedra as well as coupled vibrations of the organic and inorganic sublattices. This strong and coherent carrier–lattice coupling is resolved on femtosecond timescales and found to be important both for resonant and far–above–gap photoexcitation. As a result, this study indicates that ultrafast lattice distortions play a key role in the initial processes associated with charge transport.« less

Vibronic coupling explains the ultrafast carotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

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

Perlík, Václav; Seibt, Joachim; Šanda, František

The initial energy transfer steps in photosynthesis occur on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that Förster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which lead to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited states as part of the system’s Hamiltonian, reproduces all measuredmore » quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels on the carotenoid electronic ground state play the central role in the excited state population transfer to bacteriochlorophyll; resonance between the donor-acceptor energy gap and the vibrational ground state energies is the physical basis of the ultrafast energy transfer rates in these systems.« less

Electronic damping of anharmonic adsorbate vibrations at metallic surfaces

NASA Astrophysics Data System (ADS)

Tremblay, Jean Christophe; Monturet, Serge; Saalfrank, Peter

2010-03-01

The nonadiabatic coupling of an adsorbate close to a metallic surface leads to electronic damping of adsorbate vibrations and line broadening in vibrational spectroscopy. Here, a perturbative treatment of the electronic contribution to the lifetime broadening serves as a building block for a new approach, in which anharmonic vibrational transition rates are calculated from a position-dependent coupling function. Different models for the coupling function will be tested, all related to embedding theory. The first two are models based on a scattering approach with (i) a jellium-type and (ii) a density functional theory based embedding density, respectively. In a third variant a further refined model is used for the embedding density, and a semiempirical approach is taken in which a scaling factor is chosen to match harmonic, single-site, first-principles transition rates, obtained from periodic density functional theory. For the example of hydrogen atoms on (adsorption) and below (subsurface absorption) a Pd(111) surface, lifetimes of and transition rates between vibrational levels are computed. The transition rates emerging from different models serve as input for the selective subsurface adsorption of hydrogen in palladium starting from an adsorption site, by using sequences of infrared laser pulses in a laser distillation scheme.

Autonomous target recognition using remotely sensed surface vibration measurements

NASA Astrophysics Data System (ADS)

Geurts, James; Ruck, Dennis W.; Rogers, Steven K.; Oxley, Mark E.; Barr, Dallas N.

1993-09-01

The remotely measured surface vibration signatures of tactical military ground vehicles are investigated for use in target classification and identification friend or foe (IFF) systems. The use of remote surface vibration sensing by a laser radar reduces the effects of partial occlusion, concealment, and camouflage experienced by automatic target recognition systems using traditional imagery in a tactical battlefield environment. Linear Predictive Coding (LPC) efficiently represents the vibration signatures and nearest neighbor classifiers exploit the LPC feature set using a variety of distortion metrics. Nearest neighbor classifiers achieve an 88 percent classification rate in an eight class problem, representing a classification performance increase of thirty percent from previous efforts. A novel confidence figure of merit is implemented to attain a 100 percent classification rate with less than 60 percent rejection. The high classification rates are achieved on a target set which would pose significant problems to traditional image-based recognition systems. The targets are presented to the sensor in a variety of aspects and engine speeds at a range of 1 kilometer. The classification rates achieved demonstrate the benefits of using remote vibration measurement in a ground IFF system. The signature modeling and classification system can also be used to identify rotary and fixed-wing targets.

Terahertz vibrational signature of bacterial spores arising from nanostructure decorated endospore surface.

PubMed

Datta, Debopam; Stroscio, Michael A; Dutta, Mitra; Zhang, Weidong; Brown, Elliott R

2018-05-03

This theoretical effort is the first to explore the possible hypothesis that terahertz optical activity of Bacillus spores arises from normal vibrational modes of spore coat subcomponents in the terahertz frequency range. Bacterial strains like Bacillus and Clostridium form spores with a hardened coating made of peptidoglycan to protect its genetic material in harsh conditions. In recent years, electron microscopy and atomic force microscopy has revealed that bacterial spore surfaces are decorated with nanocylinders and honeycomb nanostructures. In this article, a simple elastic continuum model is used to describe the vibration of these nanocylinders mainly in Bacillus subtilis, which also leads to the conclusion that the terahertz signature of these spores arises from the vibration of these nanostructures. Three vibrating modes: radial/longitudinal, torsional and flexural, have been identified and discussed for the nanocylinders. The effect of bound water, which shifts the vibration frequency, is also discussed. The peptidoglycan molecule consists of polar and charged amino acids; hence, the sporal surface local vibrations interact strongly with the terahertz radiation. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultrafast dark-field surface inspection with hybrid-dispersion laser scanning

NASA Astrophysics Data System (ADS)

Yazaki, Akio; Kim, Chanju; Chan, Jacky; Mahjoubfar, Ata; Goda, Keisuke; Watanabe, Masahiro; Jalali, Bahram

2014-06-01

High-speed surface inspection plays an important role in industrial manufacturing, safety monitoring, and quality control. It is desirable to go beyond the speed limitation of current technologies for reducing manufacturing costs and opening a new window onto a class of applications that require high-throughput sensing. Here, we report a high-speed dark-field surface inspector for detection of micrometer-sized surface defects that can travel at a record high speed as high as a few kilometers per second. This method is based on a modified time-stretch microscope that illuminates temporally and spatially dispersed laser pulses on the surface of a fast-moving object and detects scattered light from defects on the surface with a sensitive photodetector in a dark-field configuration. The inspector's ability to perform ultrafast dark-field surface inspection enables real-time identification of difficult-to-detect features on weakly reflecting surfaces and hence renders the method much more practical than in the previously demonstrated bright-field configuration. Consequently, our inspector provides nearly 1000 times higher scanning speed than conventional inspectors. To show our method's broad utility, we demonstrate real-time inspection of the surface of various objects (a non-reflective black film, transparent flexible film, and reflective hard disk) for detection of 10 μm or smaller defects on a moving target at 20 m/s within a scan width of 25 mm at a scan rate of 90.9 MHz. Our method holds promise for improving the cost and performance of organic light-emitting diode displays for next-generation smart phones, lithium-ion batteries for green electronics, and high-efficiency solar cells.

Ultrafast FADC multiplexer

NASA Astrophysics Data System (ADS)

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

2002-10-01

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

Engine classification using vibrations measured by Laser Doppler Vibrometer on different surfaces

NASA Astrophysics Data System (ADS)

Wei, J.; Liu, Chi-Him; Zhu, Zhigang; Vongsy, Karmon; Mendoza-Schrock, Olga

2015-05-01

In our previous studies, vehicle surfaces' vibrations caused by operating engines measured by Laser Doppler Vibrometer (LDV) have been effectively exploited in order to classify vehicles of different types, e.g., vans, 2-door sedans, 4-door sedans, trucks, and buses, as well as different types of engines, such as Inline-four engines, V-6 engines, 1-axle diesel engines, and 2-axle diesel engines. The results are achieved by employing methods based on an array of machine learning classifiers such as AdaBoost, random forests, neural network, and support vector machines. To achieve effective classification performance, we seek to find a more reliable approach to pick authentic vibrations of vehicle engines from a trustworthy surface. Compared with vibrations directly taken from the uncooperative vehicle surfaces that are rigidly connected to the engines, these vibrations are much weaker in magnitudes. In this work we conducted a systematic study on different types of objects. We tested different types of engines ranging from electric shavers, electric fans, and coffee machines among different surfaces such as a white board, cement wall, and steel case to investigate the characteristics of the LDV signals of these surfaces, in both the time and spectral domains. Preliminary results in engine classification using several machine learning algorithms point to the right direction on the choice of type of object surfaces to be planted for LDV measurements.

Vibration characteristics of aluminum surface subjected to ultrasonic waves and their effect on wetting behavior of solder droplets.

PubMed

Ma, Lin; Xu, Zhiwu; Zheng, Kun; Yan, Jiuchun; Yang, Shiqin

2014-03-01

The vibration characteristics of an aluminum surface subjected to ultrasonic waves were investigated with a combination of numerical simulation and experimental testing. The wetting behavior of solder droplets on the vibrating aluminum surface was also examined. The results show that the vibration pattern of the aluminum surface is inhomogeneous. The amplitude of the aluminum surface exceeds the excitation amplitude in some zones, while the amplitude decreases nearly to zero in other zones. The distribution of the zero-amplitude zones is much less dependent on the strength of the vibration than on the location of the vibration source. The surface of the liquid solder vibrates at an ultrasonic frequency that is higher than the vibration source, and the amplitude of the liquid solder is almost twice that of the aluminum surface. The vibration of the surface of the base metal (liquid solder) correlates with the oxide film removal effect. Significant removal of the oxide film can be achieved within 2s when the amplitude of the aluminum surface is higher than 5.4 μm or when the amplitude of the liquid solder surface is higher than 10.2 μm. Copyright © 2013 Elsevier B.V. All rights reserved.

N-H stretching vibrations of guanosine-cytidine base pairs in solution: ultrafast dynamics, couplings, and line shapes.

PubMed

Fidder, Henk; Yang, Ming; Nibbering, Erik T J; Elsaesser, Thomas; Röttger, Katharina; Temps, Friedrich

2013-02-07

Dynamics and couplings of N-H stretching vibrations of chemically modified guanosine-cytidine (G·C) base pairs in chloroform are investigated with linear infrared spectroscopy and ultrafast two-dimensional infrared (2D-IR) spectroscopy. Comparison of G·C absorption spectra before and after H/D exchange reveals significant N-H stretching absorption in the region from 2500 up to 3300 cm(-1). Both of the local stretching modes ν(C)(NH(2))(b) of the hydrogen-bonded N-H moiety of the cytidine NH(2) group and ν(G)(NH) of the guanosine N-H group contribute to this broad absorption band. Its complex line shape is attributed to Fermi resonances of the N-H stretching modes with combination and overtones of fingerprint vibrations and anharmonic couplings to low-frequency modes. Cross-peaks in the nonlinear 2D spectra between the 3491 cm(-1) free N-H oscillator band and the bands centered at 3145 and 3303 cm(-1) imply N-H···O═C hydrogen bond character for both of these transitions. Time evolution illustrates that the 3303 cm(-1) band is composed of a nearly homogeneous band absorbing at 3301 cm(-1), ascribed to ν(G)(NH(2))(b), and a broad inhomogeneous band peaking at 3380 cm(-1) with mainly guanosine carbonyl overtone character. Kinetics and signal strengths indicate a <0.2 ps virtually complete population transfer from the excited ν(G)(NH(2))(b) mode to the ν(G)(NH) mode at 3145 cm(-1), suggesting lifetime broadening as the dominant source for the homogeneous line shape of the 3301 cm(-1) transition. For the 3145 cm(-1) band, a 0.3 ps population lifetime was obtained.

Measurement of Nanoplasmonic Field Enhancement with Ultrafast Photoemission.

PubMed

Rácz, Péter; Pápa, Zsuzsanna; Márton, István; Budai, Judit; Wróbel, Piotr; Stefaniuk, Tomasz; Prietl, Christine; Krenn, Joachim R; Dombi, Péter

2017-02-08

Probing nanooptical near-fields is a major challenge in plasmonics. Here, we demonstrate an experimental method utilizing ultrafast photoemission from plasmonic nanostructures that is capable of probing the maximum nanoplasmonic field enhancement in any metallic surface environment. Directly measured field enhancement values for various samples are in good agreement with detailed finite-difference time-domain simulations. These results establish ultrafast plasmonic photoelectrons as versatile probes for nanoplasmonic near-fields.

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

Surface Acoustic Wave Vibration Sensors for Measuring Aircraft Flutter

NASA Technical Reports Server (NTRS)

Wilson, William C.; Moore, Jason P.; Juarez, Peter D.

2016-01-01

Under NASA's Advanced Air Vehicles Program the Advanced Air Transport Technology (AATT) Project is investigating flutter effects on aeroelastic wings. To support that work a new method for measuring vibrations due to flutter has been developed. The method employs low power Surface Acoustic Wave (SAW) sensors. To demonstrate the ability of the SAW sensor to detect flutter vibrations the sensors were attached to a Carbon fiber-reinforced polymer (CFRP) composite panel which was vibrated at six frequencies from 1Hz to 50Hz. The SAW data was compared to accelerometer data and was found to resemble sine waves and match each other closely. The SAW module design and results from the tests are presented here.

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 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.

Two-color vibrational, femtosecond, fully resonant electronically enhanced CARS (FREE-CARS) of gas-phase nitric oxide.

PubMed

Stauffer, Hans U; Roy, Sukesh; Schmidt, Jacob B; Wrzesinski, Paul J; Gord, James R

2016-09-28

A resonantly enhanced, two-color, femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) approach is demonstrated and used to explore the nature of the frequency- and time-dependent signals produced by gas-phase nitric oxide (NO). Through careful selection of the input pulse wavelengths, this fully resonant electronically enhanced CARS (FREE-CARS) scheme allows rovibronic-state-resolved observation of time-dependent rovibrational wavepackets propagating on the vibrationally excited ground-state potential energy surface of this diatomic species. Despite the use of broadband, ultrafast time-resolved input pulses, high spectral resolution of gas-phase rovibronic transitions is observed in the FREE-CARS signal, dictated by the electronic dephasing timescales of these states. Analysis and computational simulation of the time-dependent spectra observed as a function of pump-Stokes and Stokes-probe delays provide insight into the rotationally resolved wavepacket motion observed on the excited-state and vibrationally excited ground-state potential energy surfaces of NO, respectively.

Ultrafast Beam Switching Using Coupled VCSELs

NASA Technical Reports Server (NTRS)

Ning, Cun-Zheng; Goorjian, Peter

2001-01-01

We propose a new approach to performing ultrafast beam switching using two coupled Vertical-Cavity Surface-Emitting Lasers (VCSELs). The strategy is demonstrated by numerical simulation, showing a beam switching of 10 deg at 42 GHz.

Nonlinear Acoustic Landmine Detection: Profiling Soil Surface Vibrations and Modeling Mesoscopic Elastic Behavior

DTIC Science & Technology

2007-05-04

TITLE AND SUBTITLE Nonlinear Acoustic Landmine Detection: Profiling Soil Surface Vibrations and Modeling Mesoscopic Elastic Behavior 6. AUTHOR(S...project report; no. 352 (2007) NONLINEAR ACOUSTIC LANDMINE DETECTION: PROFILING SOIL SURFACE VIBRATIONS AND MODELING MESOSCOPIC ELASTIC... model (Caughey 1966). Nonlinear acoustic landmine detection experiments are performed in the anechoic chamber facility using both a buried acrylic

Bacterial Adhesion on the Titanium and Stainless-Steel Surfaces Undergone Two Different Treatment Methods: Polishing and Ultrafast Laser Treatment

NASA Astrophysics Data System (ADS)

Chik, N.; Zain, W. S. Wan Md; Mohamad, A. J.; Sidek, M. Z.; Ibrahim, W. H. Wan; Reif, A.; Rakebrandt, J. H.; Pfleging, W.; Liu, X.

2018-05-01

Bacterial adhesion has become a significant problem in many industries causing billions of dollars for its complicated removal treatment and maintenance. In this study, metal surfaces undergone treatment with ultrafast laser with varies power. The microstructure produced on its original surfaces were expected to prevent the adhesion of Escherichia coli (E. coli) ATCC 8739 and Staphylococcus aureus (S. aureus) ATCC 6838. The laser treatment was performed at 380 fs pulse duration, 515 µm central wavelength and a repetition rate of 200 kHz. Stainless steel AISI 316L was treated with an average laser power of 0.04 W (SS-0.04) and 0.11 W (SS-0.11), while Grade 5 titanium alloy was tested with high laser power 0.11 W (T-0.11). The adhesion was observed after 16 hours and the number of adhering bacteria was counted per cm2. The result achieved shows that, increasing the average laser power is leading to an enhanced S. aureus adhesion while E. coli adhesion is reduced which is due to the hydrophobicity interaction and difference in surface texture. Meanwhile, the laser treatment showed significant reduction of the bacterial adhesion on its surface compared to the polished surfaces. Thus, ultrafast laser texturing can be suggested as a promising method to reduce the bacterial adhesion, which reduced the adhesion of >80% for E. coli and >20% for S. aureus.

4D multiple-cathode ultrafast electron microscopy

PubMed Central

Baskin, John Spencer; Liu, Haihua; Zewail, Ahmed H.

2014-01-01

Four-dimensional multiple-cathode ultrafast electron microscopy is developed to enable the capture of multiple images at ultrashort time intervals for a single microscopic dynamic process. The dynamic process is initiated in the specimen by one femtosecond light pulse and probed by multiple packets of electrons generated by one UV laser pulse impinging on multiple, spatially distinct, cathode surfaces. Each packet is distinctly recorded, with timing and detector location controlled by the cathode configuration. In the first demonstration, two packets of electrons on each image frame (of the CCD) probe different times, separated by 19 picoseconds, in the evolution of the diffraction of a gold film following femtosecond heating. Future elaborations of this concept to extend its capabilities and expand the range of applications of 4D ultrafast electron microscopy are discussed. The proof-of-principle demonstration reported here provides a path toward the imaging of irreversible ultrafast phenomena of materials, and opens the door to studies involving the single-frame capture of ultrafast dynamics using single-pump/multiple-probe, embedded stroboscopic imaging. PMID:25006261

4D multiple-cathode ultrafast electron microscopy.

PubMed

Baskin, John Spencer; Liu, Haihua; Zewail, Ahmed H

2014-07-22

Four-dimensional multiple-cathode ultrafast electron microscopy is developed to enable the capture of multiple images at ultrashort time intervals for a single microscopic dynamic process. The dynamic process is initiated in the specimen by one femtosecond light pulse and probed by multiple packets of electrons generated by one UV laser pulse impinging on multiple, spatially distinct, cathode surfaces. Each packet is distinctly recorded, with timing and detector location controlled by the cathode configuration. In the first demonstration, two packets of electrons on each image frame (of the CCD) probe different times, separated by 19 picoseconds, in the evolution of the diffraction of a gold film following femtosecond heating. Future elaborations of this concept to extend its capabilities and expand the range of applications of 4D ultrafast electron microscopy are discussed. The proof-of-principle demonstration reported here provides a path toward the imaging of irreversible ultrafast phenomena of materials, and opens the door to studies involving the single-frame capture of ultrafast dynamics using single-pump/multiple-probe, embedded stroboscopic imaging.

Surface sum-frequency vibrational spectroscopy of nonpolar media

DOE PAGES

Sun, Shumei; Tian, Chuanshan; Shen, Y. Ron

2015-04-27

Sum-frequency generation spectroscopy is surface specific only if the bulk contribution to the signal is negligible. Negligible bulk contribution is, however, not necessarily true, even for media with inversion symmetry. The inevitable challenge is to find the surface spectrum in the presence of bulk contribution, part of which has been believed to be inseparable from the surface contribution. Here, we show that, for nonpolar media, it is possible to separately deduce surface and bulk spectra from combined phase-sensitive sum-frequency vibrational spectroscopic measurements in reflection and transmission. Finally, the study of benzene interfaces is presented as an example.

Evaluation of selected sidewalk pavement surfaces for vibration experienced by users of manual and powered wheelchairs.

PubMed

Cooper, Rory A; Wolf, Erik; Fitzgerald, Shirley G; Kellerher, Annmarie; Ammer, William; Boninger, Michael L; Cooper, Rosemarie

2004-01-01

Obstacles such as bumps, curb descents, and uneven driving surfaces cause vibrations that affect the wheelchair, and in turn, the wheelchair user. Chronic exposure can cause low-back pain, disk degeneration, and other harmful effects. Little research has been conducted to assess the vibrations experienced by wheelchair users. The purpose of this study was to conduct an evaluation of the vibration exposure during electric-powered wheelchair driving and mechanical energy requirements for manual wheelchair propulsion over selected sidewalk surfaces. The goal was to determine the criteria for a wheelchair-pedestrian access route that does not require excessive propulsive work or expose wheelchair users to potentially harmful vibrations. Ten unimpaired individuals participated in this study. Six sidewalk surfaces were tested. Measured variables included power of the acceleration per octave, mechanical work to propel over surfaces, peak acceleration, and frequency at which peak acceleration occurs. For both the manual and electric-powered wheelchair, at 1 m/s, significant differences were found in peak accelerations between the seat and footrest (P < 0.0001) and between the sidewalk surfaces (P = 0.004). The greatest risk for injury caused by shock and vibration exposure occurs at frequencies near the natural frequency of seated humans (4-15 Hz). The values for work required to propel over the surfaces tested were not statistically significantly different. Besides appearance and construction, the only distinguishing characteristic was surface roughness caused by the joints. When treating the poured concrete sidewalk as the standard, surfaces 2, 3, 5, and 6 compared most favorably in terms of vibration exposure, whereas surface 4 produced mixed results. Surfaces 2, 3, 5, and 6 yielded results that were similar to the poured concrete sidewalk and could be considered acceptable for wheelchair users. In conclusion, surfaces other than the traditional poured concrete can be

Lateral hopping of CO molecules on Pt(111) surface by femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Hayashi, M.; Ootsuka, Y.; Paulsson, M.; Persson, B. N. J.; Ueba, H.

2009-12-01

Theory of heat transfer between adsorbate vibrational degrees of freedom and ultrafast laser heated hot electrons including vibrational intermode coupling is applied to calculate two-pulse correlation, laser fluence dependence and time dependence of lateral hopping of CO molecules from a step to terrace site on a stepped Pt (111) surface. The intermode coupling is a key ingredient to describe vibrational heating of the frustrated translation mode responsible for the CO hopping. The calculated results are in good agreement with the experimental results, especially if we scale down the experimentally determined absorbed fluence. It is found that CO hopping is induced by indirect heating of the FT mode by the FR mode with a strong frictional coupling to hot electrons.

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.

Characterizing interstate vibrational coherent dynamics of surface adsorbed catalysts by fourth-order 3D SFG spectroscopy

NASA Astrophysics Data System (ADS)

Li, Yingmin; Wang, Jiaxi; Clark, Melissa L.; Kubiak, Clifford P.; Xiong, Wei

2016-04-01

We report the first fourth-order 3D SFG spectroscopy of a monolayer of the catalyst Re(diCN-bpy)(CO)3Cl on a gold surface. Besides measuring the vibrational coherences of single vibrational modes, the fourth-order 3D SFG spectrum also measures the dynamics of interstate coherences and vibrational coherences states between two vibrational modes. By comparing the 3D SFG to the corresponding 2D and third-order 3D IR spectroscopy of the same molecules in solution, we found that the interstate coherences exist in both liquid and surface systems, suggesting that the interstate coherence is not disrupted by surface interactions. However, by analyzing the 3D spectral lineshape, we found that the interstate coherences also experience non-negligible homogenous dephasing dynamics that originate from surface interactions. This unique ability of determining interstate vibrational coherence dynamics of the molecular monolayer can help in understanding of how energy flows within surface catalysts and other molecular monolayers.

Ultrafast demagnetisation dependence on film thickness: A TDDFT calculation

NASA Astrophysics Data System (ADS)

Singh, N.; Sharma, S.

2018-04-01

Ferromagnetic materials when subjected to intense laser pulses leads to reduction of their magnetisation on an ultrafast scale. Here, we perform an ab-initio calculation to study the behavior of ultrafast demagnetisation as a function of film thickness for Nickel as compared to the bulk of the material. In thin films surface formation results in amplification of demagnetisation with the percentage of demagnetisation depending upon the film thickness.

Driving Cell Seeding Using Vibration Induced Surface Waves

NASA Astrophysics Data System (ADS)

Li, Haiyan; Friend, James; Yeo, Leslie

2007-11-01

The ability to load cells into scaffold matrices is an important step in in-vitro cell culturing. Efficient and rapid cell seeding is however difficult and has traditionally been carried out using a static method by allowing gravity to drive the perfusion of the cell suspension into the porous scaffold. Nevertheless, due to the large capillary pressures associated with the small scaffold pore dimensions, the static cell seeding method is both slow and inefficient; the majority of cells are distributed close to the surface of the scaffold due to the inability of the fluid to penetrate deep into the scaffold. By driving the liquid into the scaffold using small amplitude surface vibrations on a piezoelectric substrate, we demonstrate that the cells can be infused much quicker (approximately 10 seconds) than if allowed to perfuse by gravity alone, which requires seeding times in excess of 30 minutes. Greater penetration of the fluid and hence the cells into the scaffold is also achieved with the vibration forcing, thus giving rise to a more uniform cell distribution within the scaffold. Moreover, we have verified that 80% of the yeast cells seeded by the surface waves remained viable.

Ultrafast optical switching in three-dimensional photonic crystals

NASA Astrophysics Data System (ADS)

Mazurenko, D. A.

2004-09-01

stop band shifts to the blue leading to large (up to 35%) changes in the reflectivity. Metallo-dielectric photonic crystals give even more possibilities for the band-tuning, since in addition to the resonance for light they posses surface plasmon resonances. The interplay of these resonances leads to unusual optical phenomena. As an example, reflected light produces an unexpected beaming in the apexes of a hexagon with a divergence angle of 8°, in our sample. This angle is too small to be attributed to a simple diffraction on the periodic lattice of core-shells but can be explained by interference between surface plasmons and propagating surface waves. Time-resolved spectra demonstrate rapid changes immediately after the arrival of the pump pulse. Ultrafast reflection changes are dramatically enhanced by the plasmon resonances, and can reach values as high as 35%. A completely different mechanism for ultrafast switching is explored, based on the excitation of coherent acoustic radial vibrations of the gold spheres. This results in a 4% modulation of the reflectivity on a subnanosecond timescale. The observed oscillation properties of our gold-shell spheres are in excellent agreement with the calculations. The described results show that the demonstrated dynamical changes in the reflectivity of a three-dimensional photonic crystal can be made both large and ultrafast and therefore may prove to be relevant for future applications.

Discovery of Cellulose Surface Layer Conformation by Nonlinear Vibrational Spectroscopy

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

Zhang, Libing; Fu, Li; Wang, Hong-fei

2017-03-14

Significant questions remain with respect to the structure and polymorphs of cellulose. These include the cellulose surface layers and the bulk crystalline core as well as the conformational differences. The Total Internal Reflection Sum Frequency Generation Vibrational Spectroscopy (TIR-SFG-VS) combined with the conventional SFG-VS (non-TIR) can help to resolve these questions by selectively characterizing the molecular structures of surface layers and the crystalline core of cellulose. From the SFG spectra in the C-H and O-H regions, we found that the surface layers of Avicel are essentially amorphous; while the surface layers of Iβ cellulose are crystalline but with different structuralmore » and spectroscopic signatures than that of its crystalline core. This work demonstrates the capacity of TIR and Non-TIR SFG-VS tools in selectively studying the structures and polymorphs of cellulose. In addition, these results also suggest that the assignments of major vibrational peaks for cellulose need to be further determined.« less

Substrate Vibrations as Promoters of Chemical Reactivity on Metal Surfaces.

PubMed

Campbell, Victoria L; Chen, Nan; Guo, Han; Jackson, Bret; Utz, Arthur L

2015-12-17

Studies exploring how vibrational energy (Evib) promotes chemical reactivity most often focus on molecular reagents, leaving the role of substrate atom motion in heterogeneous interfacial chemistry underexplored. This combined theoretical and experimental study of methane dissociation on Ni(111) shows that lattice atom motion modulates the reaction barrier height during each surface atom's vibrational period, which leads to a strong variation in the reaction probability (S0) with surface temperature (Tsurf). State-resolved beam-surface scattering studies at Tsurf = 90 K show a sharp threshold in S0 at translational energy (Etrans) = 42 kJ/mol. When Etrans decreases from 42 kJ/mol to 34 kJ/mol, S0 decreases 1000-fold at Tsurf = 90 K, but only 2-fold at Tsurf = 475 K. Results highlight the mechanism for this effect, provide benchmarks for DFT calculations, and suggest the potential importance of surface atom induced barrier height modulation in heterogeneously catalyzed reactions, particularly on structurally labile nanoscale particles and defect sites.

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

PubMed

Kraack, Jan Philip

2017-10-25

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

Localized surface plasmon resonances in nanostructures to enhance nonlinear vibrational spectroscopies: towards an astonishing molecular sensitivity

PubMed Central

2014-01-01

Summary Vibrational transitions contain some of the richest fingerprints of molecules and materials, providing considerable physicochemical information. Vibrational transitions can be characterized by different spectroscopies, and alternatively by several imaging techniques enabling to reach sub-microscopic spatial resolution. In a quest to always push forward the detection limit and to lower the number of needed vibrational oscillators to get a reliable signal or imaging contrast, surface plasmon resonances (SPR) are extensively used to increase the local field close to the oscillators. Another approach is based on maximizing the collective response of the excited vibrational oscillators through molecular coherence. Both features are often naturally combined in vibrational nonlinear optical techniques. In this frame, this paper reviews the main achievements of the two most common vibrational nonlinear optical spectroscopies, namely surface-enhanced sum-frequency generation (SE-SFG) and surface-enhanced coherent anti-Stokes Raman scattering (SE-CARS). They can be considered as the nonlinear counterpart and/or combination of the linear surface-enhanced infrared absorption (SEIRA) and surface-enhanced Raman scattering (SERS) techniques, respectively, which are themselves a branching of the conventional IR and spontaneous Raman spectroscopies. Compared to their linear equivalent, those nonlinear vibrational spectroscopies have proved to reach higher sensitivity down to the single molecule level, opening the way to astonishing perspectives for molecular analysis. PMID:25551056

Non-contact measurement of facial surface vibration patterns during singing by scanning laser Doppler vibrometer.

PubMed

Kitamura, Tatsuya; Ohtani, Keisuke

2015-01-01

This paper presents a method of measuring the vibration patterns on facial surfaces by using a scanning laser Doppler vibrometer (LDV). The surfaces of the face, neck, and body vibrate during phonation and, according to Titze (2001), these vibrations occur when aerodynamic energy is efficiently converted into acoustic energy at the glottis. A vocalist's vibration velocity patterns may therefore indicate his or her phonatory status or singing skills. LDVs enable laser-based non-contact measurement of the vibration velocity and displacement of a certain point on a vibrating object, and scanning LDVs permit multipoint measurements. The benefits of scanning LDVs originate from the facts that they do not affect the vibrations of measured objects and that they can rapidly measure the vibration patterns across planes. A case study is presented herein to demonstrate the method of measuring vibration velocity patterns with a scanning LDV. The objective of the experiment was to measure the vibration velocity differences between the modal and falsetto registers while three professional soprano singers sang sustained vowels at four pitch frequencies. The results suggest that there is a possibility that pitch frequency are correlated with vibration velocity. However, further investigations are necessary to clarify the relationships between vibration velocity patterns and phonation status and singing skills.

Non-contact measurement of facial surface vibration patterns during singing by scanning laser Doppler vibrometer

PubMed Central

Kitamura, Tatsuya; Ohtani, Keisuke

2015-01-01

This paper presents a method of measuring the vibration patterns on facial surfaces by using a scanning laser Doppler vibrometer (LDV). The surfaces of the face, neck, and body vibrate during phonation and, according to Titze (2001), these vibrations occur when aerodynamic energy is efficiently converted into acoustic energy at the glottis. A vocalist's vibration velocity patterns may therefore indicate his or her phonatory status or singing skills. LDVs enable laser-based non-contact measurement of the vibration velocity and displacement of a certain point on a vibrating object, and scanning LDVs permit multipoint measurements. The benefits of scanning LDVs originate from the facts that they do not affect the vibrations of measured objects and that they can rapidly measure the vibration patterns across planes. A case study is presented herein to demonstrate the method of measuring vibration velocity patterns with a scanning LDV. The objective of the experiment was to measure the vibration velocity differences between the modal and falsetto registers while three professional soprano singers sang sustained vowels at four pitch frequencies. The results suggest that there is a possibility that pitch frequency are correlated with vibration velocity. However, further investigations are necessary to clarify the relationships between vibration velocity patterns and phonation status and singing skills. PMID:26579054

Surface morphology effects in a vibration based triboelectric energy harvester

NASA Astrophysics Data System (ADS)

Nafari, A.; Sodano, H. A.

2018-01-01

Despite the abundance of ambient mechanical energy in our environment, it is often neglected and left unused. However, recent studies have demonstrated that mechanical vibrations can be harvested and used to power small wireless electronic devices, such as micro electromechanical sensors (MEMS) and actuators. Most commonly, these energy harvesters convert vibration into electrical energy by utilizing piezoelectric, electromagnetic or electrostatic effects. Recently, triboelectric based energy harvesters have shown to be among the simplest and most cost-effective techniques for scavenging mechanical energy. The basis of triboelectric energy harvesters is the periodic contact and separation of two surfaces with opposite triboelectric properties which results in induced charge flow through an external load. Here, a vibration driven triboelectric nanogenerator (TENG) is fabricated and the effect of micro/nano scale surface modification is studied. The TENG produces electrical energy on the basis of periodic out-of-plane charge separation between gold and polydimethylsiloxane (PDMS) with opposite triboelectric charge polarities. By introducing micro/nano scale surface modifications to the PDMS and gold, the TENG’s power output is further enhanced. This work demonstrates that the morphology of the surfaces in a TENG device is important and by increasing the effective surface area through micro/nano scale modification, the power output of the device can increase by 118%. Moreover, it is shown that unlike many TENGs proposed in the literature, the fabricated device has a high RMS open circuit voltage and short circuit current and can perform for an extended period of time.

Quantification of Acute Vocal Fold Epithelial Surface Damage with Increasing Time and Magnitude Doses of Vibration Exposure

PubMed Central

Kojima, Tsuyoshi; Van Deusen, Mark; Jerome, W. Gray; Garrett, C. Gaelyn; Sivasankar, M. Preeti; Novaleski, Carolyn K.; Rousseau, Bernard

2014-01-01

Because the vocal folds undergo repeated trauma during continuous cycles of vibration, the epithelium is routinely susceptible to damage during phonation. Excessive and prolonged vibration exposure is considered a significant predisposing factor in the development of vocal fold pathology. The purpose of the present study was to quantify the extent of epithelial surface damage following increased time and magnitude doses of vibration exposure using an in vivo rabbit phonation model. Forty-five New Zealand white breeder rabbits were randomized to nine groups and received varying phonation time-doses (30, 60, or 120 minutes) and magnitude-doses (control, modal intensity phonation, or raised intensity phonation) of vibration exposure. Scanning electron microscopy and transmission electron microscopy was used to quantify the degree of epithelial surface damage. Results revealed a significant reduction in microprojection density, microprojection height, and depth of the epithelial surface with increasing time and phonation magnitudes doses, signifying increased epithelial surface damage risk with excessive and prolonged vibration exposure. Destruction to the epithelial cell surface may provide significant insight into the disruption of cell function following prolonged vibration exposure. One important goal achieved in the present study was the quantification of epithelial surface damage using objective imaging criteria. These data provide an important foundation for future studies of long-term tissue recovery from excessive and prolonged vibration exposure. PMID:24626217

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

PubMed

Fushitani, Mizuho; Hishikawa, Akiyoshi

2016-11-01

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

Ultrafast non-radiative dynamics of atomically thin MoSe 2

DOE PAGES

Lin, Ming -Fu; Kochat, Vidya; Krishnamoorthy, Aravind; ...

2017-10-17

Non-radiative energy dissipation in photoexcited materials and resulting atomic dynamics provide a promising pathway to induce structural phase transitions in two-dimensional materials. However, these dynamics have not been explored in detail thus far because of incomplete understanding of interaction between the electronic and atomic degrees of freedom, and a lack of direct experimental methods to quantify real-time atomic motion and lattice temperature. Here, we explore the ultrafast conversion of photoenergy to lattice vibrations in a model bi-layered semiconductor, molybdenum diselenide, MoSe 2. Specifically, we characterize sub-picosecond lattice dynamics initiated by the optical excitation of electronic charge carriers in the highmore » electron-hole plasma density regime. Our results focuses on the first ten picosecond dynamics subsequent to photoexcitation before the onset of heat transfer to the substrate, which occurs on a ~100 picosecond time scale. Photoinduced atomic motion is probed by measuring the time dependent Bragg diffraction of a delayed mega-electronvolt femtosecond electron beam. Transient lattice temperatures are characterized through measurement of Bragg peak intensities and calculation of the Debye-Waller factor (DWF). These measurements show a sub-picosecond decay of Bragg diffraction and a correspondingly rapid rise in lattice temperatures. We estimate a high quantum yield for the conversion of excited charge carrier energy to lattice motion under our experimental conditions, indicative of a strong electron-phonon interaction. First principles nonadiabatic quantum molecular dynamics simulations (NAQMD) on electronically excited MoSe 2 bilayers reproduce the observed picosecond-scale increase in lattice temperature and ultrafast conversion of photoenergy to lattice vibrations. Calculation of excited-state phonon dispersion curves suggests that softened vibrational modes in the excited state are involved in efficient and rapid energy

Ultrafast non-radiative dynamics of atomically thin MoSe 2

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

Lin, Ming -Fu; Kochat, Vidya; Krishnamoorthy, Aravind

Non-radiative energy dissipation in photoexcited materials and resulting atomic dynamics provide a promising pathway to induce structural phase transitions in two-dimensional materials. However, these dynamics have not been explored in detail thus far because of incomplete understanding of interaction between the electronic and atomic degrees of freedom, and a lack of direct experimental methods to quantify real-time atomic motion and lattice temperature. Here, we explore the ultrafast conversion of photoenergy to lattice vibrations in a model bi-layered semiconductor, molybdenum diselenide, MoSe 2. Specifically, we characterize sub-picosecond lattice dynamics initiated by the optical excitation of electronic charge carriers in the highmore » electron-hole plasma density regime. Our results focuses on the first ten picosecond dynamics subsequent to photoexcitation before the onset of heat transfer to the substrate, which occurs on a ~100 picosecond time scale. Photoinduced atomic motion is probed by measuring the time dependent Bragg diffraction of a delayed mega-electronvolt femtosecond electron beam. Transient lattice temperatures are characterized through measurement of Bragg peak intensities and calculation of the Debye-Waller factor (DWF). These measurements show a sub-picosecond decay of Bragg diffraction and a correspondingly rapid rise in lattice temperatures. We estimate a high quantum yield for the conversion of excited charge carrier energy to lattice motion under our experimental conditions, indicative of a strong electron-phonon interaction. First principles nonadiabatic quantum molecular dynamics simulations (NAQMD) on electronically excited MoSe 2 bilayers reproduce the observed picosecond-scale increase in lattice temperature and ultrafast conversion of photoenergy to lattice vibrations. Calculation of excited-state phonon dispersion curves suggests that softened vibrational modes in the excited state are involved in efficient and rapid energy

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.

Ultrafast photocurrents at the surface of the three-dimensional topological insulator Bi2Se3

PubMed Central

Braun, Lukas; Mussler, Gregor; Hruban, Andrzej; Konczykowski, Marcin; Schumann, Thomas; Wolf, Martin; Münzenberg, Markus; Perfetti, Luca; Kampfrath, Tobias

2016-01-01

Three-dimensional topological insulators are fascinating materials with insulating bulk yet metallic surfaces that host highly mobile charge carriers with locked spin and momentum. Remarkably, surface currents with tunable direction and magnitude can be launched with tailored light beams. To better understand the underlying mechanisms, the current dynamics need to be resolved on the timescale of elementary scattering events (∼10 fs). Here, we excite and measure photocurrents in the model topological insulator Bi2Se3 with a time resolution of 20 fs by sampling the concomitantly emitted broadband terahertz (THz) electromagnetic field from 0.3 to 40 THz. Strikingly, the surface current response is dominated by an ultrafast charge transfer along the Se–Bi bonds. In contrast, photon-helicity-dependent photocurrents are found to be orders of magnitude smaller than expected from generation scenarios based on asymmetric depopulation of the Dirac cone. Our findings are of direct relevance for broadband optoelectronic devices based on topological-insulator surface currents. PMID:27796297

The separation of vibrational coherence from ground- and excited-electronic states in P3HT film

NASA Astrophysics Data System (ADS)

Song, Yin; Hellmann, Christoph; Stingelin, Natalie; Scholes, Gregory D.

2015-06-01

Concurrence of the vibrational coherence and ultrafast electron transfer has been observed in polymer/fullerene blends. However, it is difficult to experimentally investigate the role that the excited-state vibrational coherence plays during the electron transfer process since vibrational coherence from the ground- and excited-electronic states is usually temporally and spectrally overlapped. Here, we performed 2-dimensional electronic spectroscopy (2D ES) measurements on poly(3-hexylthiophene) (P3HT) films. By Fourier transforming the whole 2D ES datasets ( S ( λ 1 , T ˜ 2 , λ 3 ) ) along the population time ( T ˜ 2 ) axis, we develop and propose a protocol capable of separating vibrational coherence from the ground- and excited-electronic states in 3D rephasing and nonrephasing beating maps ( S ( λ 1 , ν ˜ 2 , λ 3 ) ). We found that the vibrational coherence from pure excited electronic states appears at positive frequency ( + ν ˜ 2 ) in the rephasing beating map and at negative frequency ( - ν ˜ 2 ) in the nonrephasing beating map. Furthermore, we also found that vibrational coherence from excited electronic state had a long dephasing time of 244 fs. The long-lived excited-state vibrational coherence indicates that coherence may be involved in the electron transfer process. Our findings not only shed light on the mechanism of ultrafast electron transfer in organic photovoltaics but also are beneficial for the study of the coherence effect on photoexcited dynamics in other systems.

WE-B-210-02: The Advent of Ultrafast Imaging in Biomedical Ultrasound

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

Tanter, M.

In the last fifteen years, the introduction of plane or diverging wave transmissions rather than line by line scanning focused beams has broken the conventional barriers of ultrasound imaging. By using such large field of view transmissions, the frame rate reaches the theoretical limit of physics dictated by the ultrasound speed and an ultrasonic map can be provided typically in tens of micro-seconds (several thousands of frames per second). Interestingly, this leap in frame rate is not only a technological breakthrough but it permits the advent of completely new ultrasound imaging modes, including shear wave elastography, electromechanical wave imaging, ultrafastmore » doppler, ultrafast contrast imaging, and even functional ultrasound imaging of brain activity (fUltrasound) introducing Ultrasound as an emerging full-fledged neuroimaging modality. At ultrafast frame rates, it becomes possible to track in real time the transient vibrations – known as shear waves – propagating through organs. Such “human body seismology” provides quantitative maps of local tissue stiffness whose added value for diagnosis has been recently demonstrated in many fields of radiology (breast, prostate and liver cancer, cardiovascular imaging, …). Today, Supersonic Imagine company is commercializing the first clinical ultrafast ultrasound scanner, Aixplorer with real time Shear Wave Elastography. This is the first example of an ultrafast Ultrasound approach surpassing the research phase and now widely spread in the clinical medical ultrasound community with an installed base of more than 1000 Aixplorer systems in 54 countries worldwide. For blood flow imaging, ultrafast Doppler permits high-precision characterization of complex vascular and cardiac flows. It also gives ultrasound the ability to detect very subtle blood flow in very small vessels. In the brain, such ultrasensitive Doppler paves the way for fUltrasound (functional ultrasound imaging) of brain activity with

Dynamics of liquid films exposed to high-frequency surface vibration

NASA Astrophysics Data System (ADS)

Manor, Ofer; Rezk, Amgad R.; Friend, James R.; Yeo, Leslie Y.

2015-05-01

We derive a generalized equation that governs the spreading of liquid films under high-frequency (MHz-order) substrate vibration in the form of propagating surface waves and show that this single relationship is universally sufficient to collectively describe the rich and diverse dynamic phenomena recently observed for the transport of oil films under such substrate excitation, in particular, Rayleigh surface acoustic waves. In contrast to low-frequency (Hz- to kHz-order) vibration-induced wetting phenomena, film spreading at such high frequencies arises from convective drift generated by the viscous periodic flow localized in a region characterized by the viscous penetration depth β-1≡(2μ /ρ ω ) 1 /2 adjacent to the substrate that is invoked directly by its vibration; μ and ρ are the viscosity and the density of the liquid, respectively, and ω is the excitation frequency. This convective drift is responsible for driving the spreading of thin films of thickness h ≪kl-1 , which spread self-similarly as t1 /4 along the direction of the drift corresponding to the propagation direction of the surface wave, kl being the wave number of the compressional acoustic wave that forms in the liquid due to leakage of the surface wave energy from the substrate into the liquid and t the time. Films of greater thicknesses h ˜kl-1≫β-1 , in contrast, are observed to spread with constant velocity but in a direction that opposes the drift and surface wave propagation due to the attenuation of the acoustic wave in the liquid. The universal equation derived allows for the collective prediction of the spreading of these thin and thick films in opposing directions.

Picosecond vibrational spectroscopy of shocked energetic materials

NASA Astrophysics Data System (ADS)

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

1998-07-01

The dynamic response of a thin film of the insensitive high explosive 5-nitro-2,4-dihydro-3H-1,2,4-triazol-3-one (NTO) to ultrafast shock compression has been investigated by picosecond coherent anti-Stokes Raman spectroscopy (CARS). Vibrational spectra were obtained in the 1200 cm-1 to 1450 cm-1 region with a time resolution on the order of 100 ps. The frequency shifts and widths of the two vibrational transitions in this region show an entirely different behavior when subjected to a shock load of about 5 GPa. An additional weak band at 1293 cm-1 appears temporarily while the shock front is within the NTO layer.

Vibrational Surface Electron-Energy-Loss Spectroscopy Probes Confined Surface-Phonon Modes

NASA Astrophysics Data System (ADS)

Lourenço-Martins, Hugo; Kociak, Mathieu

2017-10-01

Recently, two reports [Krivanek et al. Nature (London) 514, 209 (2014), 10.1038/nature13870, Lagos et al. Nature (London) 543, 529 (2017), 10.1038/nature21699] have demonstrated the amazing possibility to probe vibrational excitations from nanoparticles with a spatial resolution much smaller than the corresponding free-space phonon wavelength using electron-energy-loss spectroscopy (EELS). While Lagos et al. evidenced a strong spatial and spectral modulation of the EELS signal over a nanoparticle, Krivanek et al. did not. Here, we show that discrepancies among different EELS experiments as well as their relation to optical near- and far-field optical experiments [Dai et al. Science 343, 1125 (2014), 10.1126/science.1246833] can be understood by introducing the concept of confined bright and dark surface phonon modes, whose density of states is probed by EELS. Such a concise formalism is the vibrational counterpart of the broadly used formalism for localized surface plasmons [Ouyang and Isaacson Philos. Mag. B 60, 481 (1989), 10.1080/13642818908205921, García de Abajo and Aizpurua Phys. Rev. B 56, 15873 (1997), 10.1103/PhysRevB.56.15873, García de Abajo and Kociak Phys. Rev. Lett. 100, 106804 (2008), 10.1103/PhysRevLett.100.106804, Boudarham and Kociak Phys. Rev. B 85, 245447 (2012), 10.1103/PhysRevB.85.245447]; it makes it straightforward to predict or interpret phenomena already known for localized surface plasmons such as environment-related energy shifts or the possibility of 3D mapping of the related surface charge densities [Collins et al. ACS Photonics 2, 1628 (2015), 10.1021/acsphotonics.5b00421].

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

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.

Vibrational dynamics of aqueous hydroxide solutions probed using broadband 2DIR spectroscopy

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

Mandal, Aritra; Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139; Tokmakoff, Andrei, E-mail: tokmakoff@uchicago.edu

2015-11-21

We employed ultrafast transient absorption and broadband 2DIR spectroscopy to study the vibrational dynamics of aqueous hydroxide solutions by exciting the O–H stretch vibrations of the strongly hydrogen-bonded hydroxide solvation shell water and probing the continuum absorption of the solvated ion between 1500 and 3800 cm{sup −1}. We observe rapid vibrational relaxation processes on 150–250 fs time scales across the entire probed spectral region as well as slower vibrational dynamics on 1–2 ps time scales. Furthermore, the O–H stretch excitation loses its frequency memory in 180 fs, and vibrational energy exchange between bulk-like water vibrations and hydroxide-associated water vibrations occursmore » in ∼200 fs. The fast dynamics in this system originate in strong nonlinear coupling between intra- and intermolecular vibrations and are explained in terms of non-adiabatic vibrational relaxation. These measurements indicate that the vibrational dynamics of the aqueous hydroxide complex are faster than the time scales reported for long-range transport of protons in aqueous hydroxide solutions.« less

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

Water Oxidation Mechanisms of Metal Oxide Catalysts by Vibrational Spectroscopy of Transient Intermediates.

PubMed

Zhang, Miao; Frei, Heinz

2017-05-05

Water oxidation is an essential reaction of an artificial photosystem for solar fuel generation because it provides electrons needed to reduce carbon dioxide or protons to a fuel. Earth-abundant metal oxides are among the most attractive catalytic materials for this reaction because of their robustness and scalability, but their efficiency poses a challenge. Knowledge of catalytic surface intermediates gained by vibrational spectroscopy under reaction conditions plays a key role in uncovering kinetic bottlenecks and provides a basis for catalyst design improvements. Recent dynamic infrared and Raman studies reveal the molecular identity of transient surface intermediates of water oxidation on metal oxides. Combined with ultrafast infrared observations of how charges are delivered to active sites of the metal oxide catalyst and drive the multielectron reaction, spectroscopic advances are poised to play a key role in accelerating progress toward improved catalysts for artificial photosynthesis.

Mode-selective vibrational modulation of charge transport in organic electronic devices

PubMed Central

Bakulin, Artem A.; Lovrincic, Robert; Yu, Xi; Selig, Oleg; Bakker, Huib J.; Rezus, Yves L. A.; Nayak, Pabitra K.; Fonari, Alexandr; Coropceanu, Veaceslav; Brédas, Jean-Luc; Cahen, David

2015-01-01

The soft character of organic materials leads to strong coupling between molecular, nuclear and electronic dynamics. This coupling opens the way to influence charge transport in organic electronic devices by exciting molecular vibrational motions. However, despite encouraging theoretical predictions, experimental realization of such approach has remained elusive. Here we demonstrate experimentally that photoconductivity in a model organic optoelectronic device can be modulated by the selective excitation of molecular vibrations. Using an ultrafast infrared laser source to create a coherent superposition of vibrational motions in a pentacene/C60 photoresistor, we observe that excitation of certain modes in the 1,500–1,700 cm−1 region leads to photocurrent enhancement. Excited vibrations affect predominantly trapped carriers. The effect depends on the nature of the vibration and its mode-specific character can be well described by the vibrational modulation of intermolecular electronic couplings. This presents a new tool for studying electron–phonon coupling and charge dynamics in (bio)molecular materials. PMID:26246039

Mode-selective vibrational modulation of charge transport in organic electronic devices

NASA Astrophysics Data System (ADS)

Bakulin, Artem A.; Lovrincic, Robert; Yu, Xi; Selig, Oleg; Bakker, Huib J.; Rezus, Yves L. A.; Nayak, Pabitra K.; Fonari, Alexandr; Coropceanu, Veaceslav; Brédas, Jean-Luc; Cahen, David

2015-08-01

The soft character of organic materials leads to strong coupling between molecular, nuclear and electronic dynamics. This coupling opens the way to influence charge transport in organic electronic devices by exciting molecular vibrational motions. However, despite encouraging theoretical predictions, experimental realization of such approach has remained elusive. Here we demonstrate experimentally that photoconductivity in a model organic optoelectronic device can be modulated by the selective excitation of molecular vibrations. Using an ultrafast infrared laser source to create a coherent superposition of vibrational motions in a pentacene/C60 photoresistor, we observe that excitation of certain modes in the 1,500-1,700 cm-1 region leads to photocurrent enhancement. Excited vibrations affect predominantly trapped carriers. The effect depends on the nature of the vibration and its mode-specific character can be well described by the vibrational modulation of intermolecular electronic couplings. This presents a new tool for studying electron-phonon coupling and charge dynamics in (bio)molecular materials.

Ultrafast formation of the benzoic acid triplet upon ultraviolet photolysis and its sequential photodissociation in solution

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

Yang Chunfan; Su Hongmei; Sun Xuezhong

2012-05-28

Time-resolved infrared (TR-IR) absorption spectroscopy in both the femtosecond and nanosecond time domain has been applied to examine the photolysis of benzoic acid in acetonitrile solution following either 267 nm or 193 nm excitation. By combining the ultrafast and nanosecond TR-IR measurements, both the excited states and the photofragments have been detected and key mechanistic insights were obtained. We show that the solvent interaction modifies the excited state relaxation pathways and thus the population dynamics, leading to different photolysis behavior in solution from that observed in the gas phase. Vibrational energy transfer to solvents dissipates excitation energy efficiently, suppressing themore » photodissociation and depopulating the excited S{sub 2} or S{sub 3} state molecules to the lowest T{sub 1} state with a rate of {approx}2.5 ps after a delayed onset of {approx}3.7 ps. Photolysis of benzoic acid using 267 nm excitation is dominated by the formation of the T{sub 1} excited state and no photofragments could be detected. The results from TR-IR experiments using higher energy of 193 nm indicate that photodissociation proceeds more rapidly than the vibrational energy transfer to solvents and C-C bond fission becomes the dominant relaxation pathway in these experiments as featured by the prominent observation of the COOH photofragments and negligible yield of the T{sub 1} excited state. The measured ultrafast formation of T{sub 1} excited state supports the existence of the surface intersections of S{sub 2}/S{sub 1}, S{sub 2}/T{sub 2}, and S{sub 1}/T{sub 1}/T{sub 2}, and the large T{sub 1} quantum yield of {approx}0.65 indicates the importance of the excited state depopulation to triplet manifold as the key factor affecting the photophysical and photochemical behavior of the monomeric benzoic acid.« less

Spectrally- and Time-Resolved Sum Frequency Generation (STiR-SFG): a new tool for ultrafast hydrogen bond dynamics at interfaces.

NASA Astrophysics Data System (ADS)

Benderskii, Alexander; Bordenyuk, Andrey; Weeraman, Champika

2006-03-01

The recently developed spectrally- and time-resolved Sum Frequency Generation (STiR-SFG) is a surface-selective 3-wave mixing (IR+visible) spectroscopic technique capable of measuring ultrafast spectral evolution of vibrational coherences. A detailed description of this measurement will be presented, and a noniterative method or deconvolving the laser pulses will be introduced to obtain the molecular response function. STiR-SFG, combined with the frequency-domain SFG spectroscopy, was applied to study hydrogen bonding dynamics at aqueous interfaces (D2O/CaF2). Spectral dynamics of the OD-stretch on the 50-150 fs time scale provides real-time observation of ultrafast H-bond rearrangement. Tuning the IR wavelength to the blue or red side of the OD-stretch transition, we selectively monitor the dynamics of different sub-ensembles in the distribution of the H-bond structures. The blue-side excitation (weaker H-bonding) shows monotonic red-shift of the OD-frequency. In contrast, the red-side excitation (stronger H-bonding structures) produces a blue-shift and a recursion, which may indicate the presence of an underdamped intermolecular mode of interfacial water. Effect of electrolyte concentration on the H-bond dynamics will be discussed.

EDITORIAL: Ultrafast magnetization processes

NASA Astrophysics Data System (ADS)

Hillebrands, Burkard

2008-09-01

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

Acoustic vibrations of metal nano-objects: Time-domain investigations

NASA Astrophysics Data System (ADS)

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

2015-01-01

Theoretical and time-domain experimental investigations of the vibrational acoustic response of nano-objects are described focusing on metallic ones. Acoustic vibrations are modeled using a macroscopic-like approach based on continuum mechanics with the proper boundary conditions, a model which yields results in excellent agreement with the experimental ones and those of atomistic calculations, down to the nanometric scale. Vibrational mode excitation and detection mechanisms and the associated mode selection in ultrafast pump-probe spectroscopy are discussed, and the measured time-dependent signals in single and ensemble of nanoparticles modeled. The launched modes, their period and their damping rate are compared to experimental results obtained on ensembles of nano-objects with different composition, morphology and environment, and with size ranging from one to hundreds of nanometers. Recent extension of time-domain spectroscopy to individual nano-objects has shed new light on the vibrational responses of isolated nanoparticles, in particular on their damping, but also raises questions on the origin of its large particle to particle dispersion.

Coherent Exciton Dynamics in the Presence of Underdamped Vibrations

DOE PAGES

Dijkstra, Arend G.; Wang, Chen; Cao, Jianshu; ...

2015-01-22

Recent ultrafast optical experiments show that excitons in large biological light-harvesting complexes are coupled to molecular vibration modes. These high-frequency vibrations will not only affect the optical response, but also drive the exciton transport. Here, using a model dimer system, the frequency of the underdamped vibration is shown to have a strong effect on the exciton dynamics such that quantum coherent oscillations in the system can be present even in the case of strong noise. Two mechanisms are identified to be responsible for the enhanced transport efficiency: critical damping due to the tunable effective strength of the coupling to themore » bath, and resonance coupling where the vibrational frequency coincides with the energy gap in the system. The interplay of these two mechanisms determines parameters responsible for the most efficient transport, and these optimal control parameters are comparable to those in realistic light-harvesting complexes. Interestingly, oscillations in the excitonic coherence at resonance are suppressed in comparison to the case of an off-resonant vibration.« less

Coherent Nuclear Wave Packets in Q States by Ultrafast Internal Conversions in Free Base Tetraphenylporphyrin.

PubMed

Kim, So Young; Joo, Taiha

2015-08-06

Persistence of vibrational coherence in electronic transition has been noted especially in biochemical systems. Here, we report the dynamics between electronic excited states in free base tetraphenylporphyrin (H2TPP) by time-resolved fluorescence with high time resolution. Following the photoexcitation of the B state, ultrafast internal conversion occurs to the Qx state directly as well as via the Qy state. Unique and distinct coherent nuclear wave packet motions in the Qx and Qy states are observed through the modulation of the fluorescence intensity in time. The instant, serial internal conversions from the B to the Qy and Qx states generate the coherent wave packets. Theory and experiment show that the observed vibrational modes involve the out-of-plane vibrations of the porphyrin ring that are strongly coupled to the internal conversion of H2TPP.

Ultrafast fluxional exchange dynamics in electrolyte solvation sheath of lithium ion battery

NASA Astrophysics Data System (ADS)

Lee, Kyung-Koo; Park, Kwanghee; Lee, Hochan; Noh, Yohan; Kossowska, Dorota; Kwak, Kyungwon; Cho, Minhaeng

2017-03-01

Lithium cation is the charge carrier in lithium-ion battery. Electrolyte solution in lithium-ion battery is usually based on mixed solvents consisting of polar carbonates with different aliphatic chains. Despite various experimental evidences indicating that lithium ion forms a rigid and stable solvation sheath through electrostatic interactions with polar carbonates, both the lithium solvation structure and more importantly fluctuation dynamics and functional role of carbonate solvent molecules have not been fully elucidated yet with femtosecond vibrational spectroscopic methods. Here we investigate the ultrafast carbonate solvent exchange dynamics around lithium ions in electrolyte solutions with coherent two-dimensional infrared spectroscopy and find that the time constants of the formation and dissociation of lithium-ion...carbonate complex in solvation sheaths are on a picosecond timescale. We anticipate that such ultrafast microscopic fluxional processes in lithium-solvent complexes could provide an important clue to understanding macroscopic mobility of lithium cation in lithium-ion battery on a molecular level.

Ultrafast fluxional exchange dynamics in electrolyte solvation sheath of lithium ion battery

PubMed Central

Lee, Kyung-Koo; Park, Kwanghee; Lee, Hochan; Noh, Yohan; Kossowska, Dorota; Kwak, Kyungwon; Cho, Minhaeng

2017-01-01

Lithium cation is the charge carrier in lithium-ion battery. Electrolyte solution in lithium-ion battery is usually based on mixed solvents consisting of polar carbonates with different aliphatic chains. Despite various experimental evidences indicating that lithium ion forms a rigid and stable solvation sheath through electrostatic interactions with polar carbonates, both the lithium solvation structure and more importantly fluctuation dynamics and functional role of carbonate solvent molecules have not been fully elucidated yet with femtosecond vibrational spectroscopic methods. Here we investigate the ultrafast carbonate solvent exchange dynamics around lithium ions in electrolyte solutions with coherent two-dimensional infrared spectroscopy and find that the time constants of the formation and dissociation of lithium-ion···carbonate complex in solvation sheaths are on a picosecond timescale. We anticipate that such ultrafast microscopic fluxional processes in lithium-solvent complexes could provide an important clue to understanding macroscopic mobility of lithium cation in lithium-ion battery on a molecular level. PMID:28272396

Ultrafast fluxional exchange dynamics in electrolyte solvation sheath of lithium ion battery.

PubMed

Lee, Kyung-Koo; Park, Kwanghee; Lee, Hochan; Noh, Yohan; Kossowska, Dorota; Kwak, Kyungwon; Cho, Minhaeng

2017-03-08

Lithium cation is the charge carrier in lithium-ion battery. Electrolyte solution in lithium-ion battery is usually based on mixed solvents consisting of polar carbonates with different aliphatic chains. Despite various experimental evidences indicating that lithium ion forms a rigid and stable solvation sheath through electrostatic interactions with polar carbonates, both the lithium solvation structure and more importantly fluctuation dynamics and functional role of carbonate solvent molecules have not been fully elucidated yet with femtosecond vibrational spectroscopic methods. Here we investigate the ultrafast carbonate solvent exchange dynamics around lithium ions in electrolyte solutions with coherent two-dimensional infrared spectroscopy and find that the time constants of the formation and dissociation of lithium-ion···carbonate complex in solvation sheaths are on a picosecond timescale. We anticipate that such ultrafast microscopic fluxional processes in lithium-solvent complexes could provide an important clue to understanding macroscopic mobility of lithium cation in lithium-ion battery on a molecular level.

The effect of inclined soil layers on surface vibration from underground railways using a semi-analytical approach

NASA Astrophysics Data System (ADS)

Jones, S.; Hunt, H.

2009-08-01

Ground vibration due to underground railways is a significant source of disturbance for people living or working near the subways. The numerical models used to predict vibration levels have inherent uncertainty which must be understood to give confidence in the predictions. A semi-analytical approach is developed herein to investigate the effect of soil layering on the surface vibration of a halfspace where both soil properties and layer inclination angles are varied. The study suggests that both material properties and inclination angle of the layers have significant effect (± 10dB) on the surface vibration response.

Enhanced Vibrational Echo Correlation Spectrometer for the Study of Molecular Dynamics, Structures, and Analytical Applications

DTIC Science & Technology

2006-09-10

ultrafast IR 2D vibrational echo spectrometer. The major improvement involved a new dual MCT array detector composed of two 32 x 1 element MCT IR... detector arrays. The dual array makes it possible to improve signal- to- noise ratio in the heterodyne detection of the vibrational echo signal. To...are dispersed in a monochromator and then detected with the new 2x32-element MCT IR array detector . As discussed above, the function of the local

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.

Ultrafast coherence transfer in DNA-templated silver nanoclusters

PubMed Central

Thyrhaug, Erling; Bogh, Sidsel Ammitzbøll; Carro-Temboury, Miguel R; Madsen, Charlotte Stahl; Vosch, Tom; Zigmantas, Donatas

2017-01-01

DNA-templated silver nanoclusters of a few tens of atoms or less have come into prominence over the last several years due to very strong absorption and efficient emission. Applications in microscopy and sensing have already been realized, however little is known about the excited-state structure and dynamics in these clusters. Here we report on a multidimensional spectroscopy investigation of the energy-level structure and the early-time relaxation cascade, which eventually results in the population of an emitting state. We find that the ultrafast intramolecular relaxation is strongly coupled to a specific vibrational mode, resulting in the concerted transfer of population and coherence between excited states on a sub-100 fs timescale. PMID:28548085

Environmentally stable seed source for high power ultrafast laser

NASA Astrophysics Data System (ADS)

Samartsev, Igor; Bordenyuk, Andrey; Gapontsev, Valentin

2017-02-01

We present an environmentally stable Yb ultrafast ring oscillator utilizing a new method of passive mode-locking. The laser is using all-fiber architecture which makes it insensitive to environmental factors, like temperature, humidity, vibrations, and shocks. The new method of mode-locking is utilizing crossed bandpass transmittance filters in ring architecture to discriminate against CW lasing. Broadband pulse evolves from cavity noise under amplification, after passing each filter, causing strong spectral broadening. The laser is self-starting. It generates transform limited spectrally flat pulses of 1 - 50 nm width at 6 - 15 MHz repetition rate and pulse energy 0.2 - 15 nJ at 1010 - 1080 nm CWL.

Whole-body vibration exposure of haul truck drivers at a surface coal mine.

PubMed

Wolfgang, Rebecca; Burgess-Limerick, Robin

2014-11-01

Haul truck drivers at surface mines are exposed to whole-body vibration for extended periods. Thirty-two whole-body vibration measurements were gathered from haul trucks under a range of normal operating conditions. Measurements taken from 30 of the 32 trucks fell within the health guidance caution zone defined by ISO2631-1 for an 8 h daily exposure suggesting, according to ISO2631-1, that "caution with respect to potential health risks is indicated". Maintained roadways were associated with substantially lower vibration amplitudes. Larger trucks were associated with lower vibration levels than small trucks. The descriptive nature of the research, and small sample size, prevents any strong conclusion regarding causal links. Further investigation of the variables associated with elevated vibration levels is justified. The operators of mining equipment such as haul trucks are exposed to whole-body vibration amplitudes which have potential to lead to long term health effects. Systematic whole-body vibration measurements taken at frequent intervals are required to provide an understanding of the causes of elevated vibration levels and hence determine appropriate control measures. Copyright © 2014 Elsevier Ltd and The Ergonomics Society. All rights reserved.

Ultrafast Adiabatic Photodehydration of 2-Hydroxymethylphenol and the Formation of Quinone Methide.

PubMed

Škalamera, Đani; Antol, Ivana; Mlinarić-Majerski, Kata; Vančik, Hrvoj; Phillips, David Lee; Ma, Jiani; Basarić, Nikola

2018-04-20

The photochemical reactivity of 2-hydroxymethylphenol (1) was investigated experimentally by photochemistry under cryogenic conditions, by detecting reactive intermediates by IR spectroscopy, and by using nanosecond and femtosecond transient absorption spectroscopic methods in solution at room temperature. In addition, theoretical studies were performed to facilitate the interpretation of the experimental results and also to simulate the reaction pathway to obtain a better understanding of the reaction mechanism. The main finding of this work is that photodehydration of 1 takes place in an ultrafast adiabatic photochemical reaction without any clear intermediate, delivering quinone methide (QM) in the excited state. Upon photoexcitation to a higher vibrational level of the singlet excited state, 1 undergoes vibrational relaxation leading to two photochemical pathways, one by which synchronous elimination of H 2 O gives QM 2 in its S 1 state and the other by which homolytic cleavage of the phenolic O-H bond produces a phenoxyl radical (S 0 ). Both are ultrafast processes that occur within a picosecond. The excited state of QM 2 (S 1 ) probably deactivates to S 0 through a conical intersection to give QM 2 (S 0 ), which subsequently delivers benzoxete 4. Elucidation of the reaction mechanisms for the photodehydration of phenols by which QMs are formed is important to tune the reactivity of QMs with DNA and proteins for the potential application of QMs in medicine as therapeutic agents. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Heterodyne-detected dispersed vibrational echo spectroscopy.

PubMed

Jones, Kevin C; Ganim, Ziad; Tokmakoff, Andrei

2009-12-24

We develop heterodyned dispersed vibrational echo spectroscopy (HDVE) and demonstrate the new capabilities in biophysical applications. HDVE is a robust ultrafast technique that provides a characterization of the real and imaginary components of third-order nonlinear signals with high sensitivity and single-laser-shot capability and can be used to extract dispersed pump-probe and dispersed vibrational echo spectra. Four methods for acquiring HDVE phase and amplitude spectra were compared: Fourier transform spectral interferometry, a new phase modulation spectral interferometry technique, and combination schemes. These extraction techniques were demonstrated in the context of protein amide I spectroscopy. Experimental HDVE and heterodyned free induction decay amide I spectra were explicitly compared to conventional dispersed pump-probe, dispersed vibrational echo, and absorption spectra. The new capabilities of HDVE were demonstrated by acquiring single-shot spectra and melting curves of ubiquitin and concentration-dependent spectra of insulin suitable for extracting the binding constant for dimerization. The introduced techniques will prove particularly useful in transient experiments, studying irreversible reactions, and micromolar concentration studies of small proteins.

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

NASA Astrophysics Data System (ADS)

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

2017-02-01

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

Isotopic effects in vibrational relaxation dynamics of H on a Si(100) surface

NASA Astrophysics Data System (ADS)

Bouakline, F.; Lorenz, U.; Melani, G.; Paramonov, G. K.; Saalfrank, P.

2017-10-01

In a recent paper [U. Lorenz and P. Saalfrank, Chem. Phys. 482, 69 (2017)], we proposed a robust scheme to set up a system-bath model Hamiltonian, describing the coupling of adsorbate vibrations (system) to surface phonons (bath), from first principles. The method is based on an embedded cluster approach, using orthogonal coordinates for system and bath modes, and an anharmonic phononic expansion of the system-bath interaction up to second order. In this contribution, we use this model Hamiltonian to calculate vibrational relaxation rates of H-Si and D-Si bending modes, coupled to a fully H(D)-covered Si(100)-( 2 × 1 ) surface, at zero temperature. The D-Si bending mode has an anharmonic frequency lying inside the bath frequency spectrum, whereas the H-Si bending mode frequency is outside the bath Debye band. Therefore, in the present calculations, we only take into account one-phonon system-bath couplings for the D-Si system and both one- and two-phonon interaction terms in the case of H-Si. The computation of vibrational lifetimes is performed with two different approaches, namely, Fermi's golden rule, and a generalized Bixon-Jortner model built in a restricted vibrational space of the adsorbate-surface zeroth-order Hamiltonian. For D-Si, the Bixon-Jortner Hamiltonian can be solved by exact diagonalization, serving as a benchmark, whereas for H-Si, an iterative scheme based on the recursive residue generation method is applied, with excellent convergence properties. We found that the lifetimes obtained with perturbation theory, albeit having almost the same order of magnitude—a few hundred fs for D-Si and a couple of ps for H-Si—, are strongly dependent on the discretized numerical representation of the bath spectral density. On the other hand, the Bixon-Jortner model is free of such numerical deficiencies, therefore providing better estimates of vibrational relaxation rates, at a very low computational cost. The results obtained with this model clearly show

Experimental study of heat transfer enhancement due to the surface vibrations in a flexible double pipe heat exchanger

NASA Astrophysics Data System (ADS)

Hosseinian, A.; Meghdadi Isfahani, A. H.

2018-04-01

In this study, the heat transfer enhancement due to the surface vibration for a double pipe heat exchanger, made of PVDF, is investigated. In order to create forced vibrations (3-9 m/s2, 100 Hz) on the outer surface of the heat exchanger electro-dynamic vibrators are used. Experiments were performed at inner Reynolds numbers ranging from 2533 to 9960. The effects of volume flow rate and temperature on heat transfer performance are evaluated. Results demonstrated that heat transfer coefficient increases by increasing vibration level and mass flow rate. The most increase in heat transfer coefficient is 97% which is obtained for the highest vibration level (9 m/s2) in the experiment range.

Receptivity of the Boundary Layer to Vibrations of the Wing Surface

NASA Astrophysics Data System (ADS)

Bernots, Tomass; Ruban, Anatoly; Pryce, David; Laminar Flow Control UK Group Team

2014-11-01

In this work we study generation of Tollmien-Schlichting (T-S) waves in the boundary layer due to elastic vibrations of the wing surface. The flow is investigated based on the asymptotic analysis of the Navier-Stokes equations at large values of the Reynolds number. It is assumed that in the spectrum of the wing vibrations there is a harmonic which comes in resonance with the T-S wave on the lower branch of the stability curve. It was found that the vibrations of the wing surface produce pressure perturbations in the flow outside the boundary layer which can be calculated with the help of the piston theory. As the pressure perturbations penetrate into the boundary layer, a Stokes layer forms on the wing surface which appears to be influenced significantly by the compressibility of the flow, and is incapable of producing the T-S waves. The situation changes when the Stokes layer encounters an roughness; near which the flow is described using the triple-deck theory. The solution of the triple-deck problem can be found in an analytic form. Our main concern is with the flow behaviour downstream of the roughness and, in particular, with the amplitude of the generated Tollmien-Schlichting waves. This research was performed in the Laminar Flow Control Centre (LFC-UK) at Imperial College London. The centre is supported by EPSRC, Airbus UK and EADS Innovation Works.

Acoustic vibrations of single suspended gold nanostructures

NASA Astrophysics Data System (ADS)

Major, Todd A.

The acoustic vibrations for single gold nanowires and gold plates were studied using time-resolved ultrafast transient absorption. The objective of this work was to remove the contribution of the supporting substrate from the damping of the acoustic vibrations of the metal nano-objects. This was achieved by suspending the nano-objects across trenches created by photolithography and reactive ion etching. Transient absorption measurements for single suspended gold nanowires were initially completed in air and water environments. The acoustic vibrations for gold nanowires over the trench in air last typically for several nanoseconds, whereas gold nanowires in water are damped more quickly. Continuum mechanics models suggest that the acoustic impedance mismatch between air and water dominates the damping rate. Later transient absorption studies on single suspended gold nanowires were completed in glycerol and ethylene glycol environments. However, our continuum mechanical model suggests nearly complete damping in glycerol due to its high viscosity, but similar damping rates are seen between the two liquids. The continuum mechanics model thus incorrectly addresses high viscosity effects on the lifetimes of the acoustic vibrations, and more complicated viscoelastic interactions occur for the higher viscosity liquids. (Abstract shortened by UMI.).

Mode-specific vibrational excitation and energy redistribution after ultrafast intramolecular electron transfer

NASA Astrophysics Data System (ADS)

Hogiu, S.; Werncke, W.; Pfeiffer, M.; Dreyer, J.; Elsaesser, T.

2000-07-01

Vibrational relaxation in the electronic ground state initiated by intramolecular back-electron transfer (b-ET) of betaine-30 (B-30) is studied by picosecond time-resolved anti-Stokes Raman spectroscopy. Measurements were carried out with B-30 dissolved in slowly as well as in rapidly relaxing solvents. We observed a risetime of the Raman band with the highest frequency near 1600 cm-1 which is close to the b-ET time τb-ET of B-30. For B-30 dissolved in propylene carbonate (τb-ET˜1 ps), the population of this mode exhibits a rise time of 1 ps whereas vibrational populations between 400 and 1400 cm-1 increase substantially slower. In contrast, in glycerol triacetin (τb-ET˜3.5 ps) and in ethanol (τb-ET˜6 ps) rise times of all modes are close to the respective b-ET times. Within the first few picoseconds, direct vibrational excitation through b-ET is favored for modes with the highest frequencies and high Franck-Condon factors. Later on, indirect channels of population due to vibrational energy redistribution (IVR) become effective. Thermal equilibrium populations of the Raman active modes are established within 10 to 15 ps after optical excitation.

Ultrafast Laser Beam Switching and Pulse Train Generation by Using Coupled Vertical-Cavity, Surface-Emitting Lasers (VCSELS)

NASA Technical Reports Server (NTRS)

Goorjian, Peter M. (Inventor); Ning, Cun-Zheng (Inventor)

2005-01-01

Ultrafast directional beam switching is achieved using coupled VCSELs. This approach is demonstrated to achieve beam switching frequencies of 40 GHz and more and switching directions of about eight degrees. This switching scheme is likely to be useful for ultrafast optical networks at frequencies much higher than achievable with other approaches.

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

PubMed

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

2017-01-11

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

Electronic and Vibrational Coherence in Charge-Transfer Reactions

NASA Astrophysics Data System (ADS)

Scherer, Norbert

1996-03-01

The ultrafast dynamics associated with optically-induced intervalence charge-transfer reactions in solution and protein environments are reported. These studies include the Fe^(II)-Fe^(III) MMCT complex Prussian blue and the mixed valence dimer (CN)_5Ru^(II)CNRuRu^(III)(NH_3)_5. The protein systems include blue copper proteins and the bacterial photosynthetic reaction center. The experimental approaches include photon echo, wavelength-resolved pump-probe and anisotropy measurements performed with 12-16fs duration optical pulses. Complicated time-domain waveforms reflect the several different p[rocesses and time scales for relaxation of coherences (both electronic and vibrational) and populations within these systems. The photon echo and anisotropy results probe electronic coherence and dephasing prior to back electron transfer. Wavelength-resolved pump-probe results reveal vibrational modes coupled to the CT-coordinate as well as formation of new product states or vibrational cooling in the ground state following back electron transfer.

Probing and controlling terahertz-driven structural dynamics with surface sensitivity

DOE PAGES

Bowlan, Pamela Renee; Bowlan, J.; Trugman, S. A.; ...

2017-03-17

Intense, single-cycle terahertz (THz) pulses are powerful tools to understand and control material properties through low-energy resonances, such as phonons. Combining this with optical second harmonic generation (SHG) makes it possible to observe the resulting ultrafast structural changes with surface sensitivity. This makes SHG an ideal method to probe phonon dynamics in topological insulators (TI), materials with unique surface transport properties. Here, we resonantly excite a phonon mode in the TI Bi 2Se 3with THz pulses and use SHG to separate the resulting symmetry changes at the surface from the bulk. Furthermore, we coherently control the lattice vibrations with amore » pair of THz pulses. Lastly, our work demonstrates a versatile, table-top tool to probe and control phonon dynamics in a range of systems, particularly at surfaces and interfaces.« less

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

PubMed

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

2013-05-03

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

Ultrafast carrier dynamics in GaN/InGaN multiple quantum wells nanorods

NASA Astrophysics Data System (ADS)

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

2018-01-01

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

Foreword: The 12th International Conference on Vibrations at Surfaces (VAS 12) (Erice, 20 26 July 2007)

NASA Astrophysics Data System (ADS)

Benedek, Giorgio; Vattuone, Luca

2008-06-01

The 12th International Conference on Vibrations at Surfaces (VAS 12) took place from 20 26 July 2007 as an event of the International School of Solid State Physics at the Ettore Majorana Foundation and Centre for Scientific Culture, Erice (Italy). The format and special environment of the conference have contributed to its transition from a traditional, medium-size conference into a more effective workshop, with a series of lectures reporting the most recent developments in the field, two poster sessions presenting recent results and even works in progress being discussed. The papers collected in this issue cover the highlights of the conference very thoroughly. Quite a few novel aspects concerning vibrations at surfaces are represented here, for example: new aspects in surface phonon spectroscopy, such as the very recent progress in inelastic x-ray scattering, the first observation of the boson peak in disordered surfaces, progress in the theory of atom scattering inelastic resonances, the action spectroscopy, the study of polycrystalline surfaces with electron energy-loss spectroscopy etc; parallel developments in experimental vibrational studies of adsorbed phases, either inorganic or organic, with those in ab initio theoretical simulations; the theory of enhanced electron--phonon interaction in low dimensions (2D and 1D); the extension from the traditional realm of surface vibrations and spectroscopy to other aspects of surface dynamics, like friction and various nonlinear effects, and to relevant dynamical phenomena occurring at interfaces. Other novelties presented at the conference, but already published in recent issues of the Journal of Physics: Condensed Matter, are also worth mentioning: the spin-echo spectroscopy with 3He allowing for slow-dynamics spectroscopy at very high, unprecedented resolutions (2007 J. Phys.: Cond. Matter 19 300301 and 305010; the first demonstration of dissociative surface trapping of molecules (2007 J. Phys.: Cond. Matter 19

Optimal placement of trailing-edge flaps for helicopter vibration reduction using response surface methods

NASA Astrophysics Data System (ADS)

Viswamurthy, S. R.; Ganguli, Ranjan

2007-03-01

This study aims to determine optimal locations of dual trailing-edge flaps to achieve minimum hub vibration levels in a helicopter, while incurring low penalty in terms of required trailing-edge flap control power. An aeroelastic analysis based on finite elements in space and time is used in conjunction with an optimal control algorithm to determine the flap time history for vibration minimization. The reduced hub vibration levels and required flap control power (due to flap motion) are the two objectives considered in this study and the flap locations along the blade are the design variables. It is found that second order polynomial response surfaces based on the central composite design of the theory of design of experiments describe both objectives adequately. Numerical studies for a four-bladed hingeless rotor show that both objectives are more sensitive to outboard flap location compared to the inboard flap location by an order of magnitude. Optimization results show a disjoint Pareto surface between the two objectives. Two interesting design points are obtained. The first design gives 77 percent vibration reduction from baseline conditions (no flap motion) with a 7 percent increase in flap power compared to the initial design. The second design yields 70 percent reduction in hub vibration with a 27 percent reduction in flap power from the initial design.

Anharmonic Effects on the Electron-Energy Spectra of Surface Vibrations

NASA Astrophysics Data System (ADS)

Ariyasu, Janice Carol

First, we consider the effect of lateral interactions on double losses and overtones in electron-energy-loss studies of surface vibrations. We develop a theory of two-phonon losses in the dipole-dominated regime of small -angle scattering. Our calculation employs the simple model of an ordered overlayer of molecules adsorbed on a crystal surface. With this model, we can identify two features; one which corresponds to the double loss and another which corresponds the excitation of an overtone. We then study the role of lateral interactions in each. We find that the presence of lateral interactions affects the position of the overtone relative to the double loss, and influences both its width and shape. The implications of these results are discussed, particularly as they relate to estimates of dissociation energies by the Birge-Sponer procedure. Next, we consider the anharmonic damping of adsorbate vibrations, with specific applications to species (S, O, and CO) adsorbed on the Ni(100) and Ni(111) surfaces. Our attention is restricted to adsorbate modes that can decay by two-phonon processes to one substrate phonon and either another substrate mode phonon or to a phonon of a mode that is localized on the adsorbate. The magnitude and temperature variation of the linewidth of adsorbate modes by this mechanism is explored; we find that near room temperature the calculated linewidths vary linearly with temperature. We also simulate the inhomogeneous broadening produced by disorder by considering the eigenfrequencies of infrared -active modes. Finally, we consider the diffuse scattering of electrons from surfaces by long-wavelength, acoustic phonons. The mechanism that we explore is the modulation of the image potential from ripples induced in the surface profile by thermally-excited surface and bulk phonons. We compare our results with earlier studies, and with the scattering produced by the dynamic-dipole moment of the surface atoms.

Vibration parameters affecting vibration-induced reflex muscle activity.

PubMed

Cidem, Muharrem; Karacan, Ilhan; Cakar, Halil Ibrahim; Cidem, Mehmet; Sebik, Oguz; Yilmaz, Gizem; Turker, Kemal Sitki; Karamehmetoglu, Safak Sahir

2017-03-01

To determine vibration parameters affecting the amplitude of the reflex activity of soleus muscle during low-amplitude whole-body vibration (WBV). This study was conducted on 19 participants. Vibration frequencies of 25, 30, 35, 40, 45, and 50 Hz were used. Surface electromyography, collision force between vibration platform and participant's heel measured using a force sensor, and acceleration measured using an accelerometer fixed to the vibration platform were simultaneously recorded. The collision force was the main independent predictor of electromyographic amplitude. The essential parameter of vibration affecting the amplitude of the reflex muscle activity is the collision force.

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.

Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging

NASA Astrophysics Data System (ADS)

Cocker, Tyler L.; Peller, Dominik; Yu, Ping; Repp, Jascha; Huber, Rupert

2016-11-01

Watching a single molecule move on its intrinsic timescale has been one of the central goals of modern nanoscience, and calls for measurements that combine ultrafast temporal resolution with atomic spatial resolution. Steady-state experiments access the requisite spatial scales, as illustrated by direct imaging of individual molecular orbitals using scanning tunnelling microscopy or the acquisition of tip-enhanced Raman and luminescence spectra with sub-molecular resolution. But tracking the intrinsic dynamics of a single molecule directly in the time domain faces the challenge that interactions with the molecule must be confined to a femtosecond time window. For individual nanoparticles, such ultrafast temporal confinement has been demonstrated by combining scanning tunnelling microscopy with so-called lightwave electronics, which uses the oscillating carrier wave of tailored light pulses to directly manipulate electronic motion on timescales faster even than a single cycle of light. Here we build on ultrafast terahertz scanning tunnelling microscopy to access a state-selective tunnelling regime, where the peak of a terahertz electric-field waveform transiently opens an otherwise forbidden tunnelling channel through a single molecular state. It thereby removes a single electron from an individual pentacene molecule’s highest occupied molecular orbital within a time window shorter than one oscillation cycle of the terahertz wave. We exploit this effect to record approximately 100-femtosecond snapshot images of the orbital structure with sub-ångström spatial resolution, and to reveal, through pump/probe measurements, coherent molecular vibrations at terahertz frequencies directly in the time domain. We anticipate that the combination of lightwave electronics and the atomic resolution of our approach will open the door to visualizing ultrafast photochemistry and the operation of molecular electronics on the single-orbital scale.

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.

Distributed ultrafast fibre laser

PubMed Central

Liu, Xueming; Cui, Yudong; Han, Dongdong; Yao, Xiankun; Sun, Zhipei

2015-01-01

A traditional ultrafast fibre laser has a constant cavity length that is independent of the pulse wavelength. The investigation of distributed ultrafast (DUF) lasers is conceptually and technically challenging and of great interest because the laser cavity length and fundamental cavity frequency are changeable based on the wavelength. Here, we propose and demonstrate a DUF fibre laser based on a linearly chirped fibre Bragg grating, where the total cavity length is linearly changeable as a function of the pulse wavelength. The spectral sidebands in DUF lasers are enhanced greatly, including the continuous-wave (CW) and pulse components. We observe that all sidebands of the pulse experience the same round-trip time although they have different round-trip distances and refractive indices. The pulse-shaping of the DUF laser is dominated by the dissipative processes in addition to the phase modulations, which makes our ultrafast laser simple and stable. This laser provides a simple, stable, low-cost, ultrafast-pulsed source with controllable and changeable cavity frequency. PMID:25765454

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

NASA Astrophysics Data System (ADS)

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

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

Ultrafast Directional Beam Switching in Coupled VCSELs

NASA Technical Reports Server (NTRS)

Ning, Cun-Zheng; Goorjian, Peter

2001-01-01

We propose a new approach to performing ultrafast directional beam switching using two coupled Vertical-Cavity Surface-Emitting Lasers (VCSELs). The proposed strategy is demonstrated for two VCSELs of 5.6 microns in diameter placed about 1 micron apart from the edges, showing a switching speed of 42 GHz with a maximum far-field angle span of about 10 degrees.

Cladding-like waveguide fabricated by cooperation of ultrafast laser writing and ion irradiation: characterization and laser generation.

PubMed

Lv, Jinman; Shang, Zhen; Tan, Yang; Vázquez de Aldana, Javier Rodríguez; Chen, Feng

2017-08-07

We report the surface cladding-like waveguide fabricated by the cooperation of the ultrafast laser writing and the ion irradiation. The ultrafast laser writes tracks near the surface of the Nd:YAG crystal, constructing a semi-circle columnar structure with a decreased refractive index of - 0.00208. Then, the Nd:YAG crystal is irradiated by the Carbon ion beam, forming an enhanced-well in the semi-circle columnar with an increased refractive index of + 0.0024. Tracks and the enhanced-well consisted a surface cladding-like waveguide. Utilizing this cladding-like waveguide as the gain medium for the waveguide lasing, optimized characterizations were observed compared with the monolayer waveguide. This work demonstrates the refractive index of the Nd:YAG crystal can be well tailored by the cooperation of the ultrafast laser writing and the ion irradiation, which provides an convenient way to fabricate the complex and multilayered photonics devices.

Roadmap on ultrafast optics

NASA Astrophysics Data System (ADS)

Reid, Derryck T.; Heyl, Christoph M.; Thomson, Robert R.; Trebino, Rick; Steinmeyer, Günter; Fielding, Helen H.; Holzwarth, Ronald; Zhang, Zhigang; Del'Haye, Pascal; Südmeyer, Thomas; Mourou, Gérard; Tajima, Toshiki; Faccio, Daniele; Harren, Frans J. M.; Cerullo, Giulio

2016-09-01

The year 2015 marked the 25th anniversary of modern ultrafast optics, since the demonstration of the first Kerr lens modelocked Ti:sapphire laser in 1990 (Spence et al 1990 Conf. on Lasers and Electro-Optics, CLEO, pp 619-20) heralded an explosion of scientific and engineering innovation. The impact of this disruptive technology extended well beyond the previous discipline boundaries of lasers, reaching into biology labs, manufacturing facilities, and even consumer healthcare and electronics. In recognition of such a milestone, this roadmap on Ultrafast Optics draws together articles from some of the key opinion leaders in the field to provide a freeze-frame of the state-of-the-art, while also attempting to forecast the technical and scientific paradigms which will define the field over the next 25 years. While no roadmap can be fully comprehensive, the thirteen articles here reflect the most exciting technical opportunities presented at the current time in Ultrafast Optics. Several articles examine the future landscape for ultrafast light sources, from practical solid-state/fiber lasers and Raman microresonators to exotic attosecond extreme ultraviolet and possibly even zeptosecond x-ray pulses. Others address the control and measurement challenges, requiring radical approaches to harness nonlinear effects such as filamentation and parametric generation, coupled with the question of how to most accurately characterise the field of ultrafast pulses simultaneously in space and time. Applications of ultrafast sources in materials processing, spectroscopy and time-resolved chemistry are also discussed, highlighting the improvements in performance possible by using lasers of higher peak power and repetition rate, or by exploiting the phase stability of emerging new frequency comb sources.

Local Environment and Interactions of Liquid and Solid Interfaces Revealed by Spectral Line Shape of Surface Selective Nonlinear Vibrational Probe

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

Chen, Shun-Li; Fu, Li; Chase, Zizwe A.

Vibrational spectral lineshape contains important detailed information of molecular vibration and reports its specific interactions and couplings to its local environment. In this work, recently developed sub-1 cm-1 high-resolution broadband sum frequency generation vibrational spectroscopy (HR-BB-SFG-VS) was used to measure the -C≡N stretch vibration in the 4-n-octyl-4’-cyanobiphenyl (8CB) Langmuir or Langmuir-Blodgett (LB) monolayer as a unique vibrational probe, and the spectral lineshape analysis revealed the local environment and interactions at the air/water, air/glass, air/calcium fluoride and air/-quartz interfaces for the first time. The 8CB Langmuir or LB film is uniform and the vibrational spectral lineshape of its -C≡N group hasmore » been well characterized, making it a good choice as the surface vibrational probe. Lineshape analysis of the 8CB -C≡N stretch SFG vibrational spectra suggests the coherent vibrational dynamics and the structural and dynamic inhomogeneity of the -C≡N group at each interface are uniquely different. In addition, it is also found that there are significantly different roles for water molecules in the LB films on different substrate surfaces. These results demonstrated the novel capabilities of the surface nonlinear spectroscopy in characterization and in understanding the specific structures and chemical interactions at the liquid and solid interfaces in general.« less

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

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

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

2014-07-01

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

Ultrafast photochemistry of polyatomic molecules containing labile halogen atoms in solution

NASA Astrophysics Data System (ADS)

Mereshchenko, Andrey S.

Because breaking and making of chemical bonds lies at the heart of chemistry, this thesis focuses on dynamic studies of labile molecules in solutions using ultrafast transient absorption spectroscopy. Specifically, my interest is two-fold: (i) novel reaction intermediates of polyhalogenated carbon, boron and phosphorus compounds; (ii) photophysics and photochemistry of labile copper(II) halide complexes. Excitation of CH2Br2, CHBr3, BBr 3, and PBr3 into n(Br)sigma*(X-Br) states, where X=C, B, or P, leads to direct photoisomerization with formation of isomers having Br-Br bonds as well as rupture of one of X-Br bonds with the formation of a Br atom and a polyatomic radical fragment, which subsequently recombine to form similar isomer products. Nonpolar solvation stabilizes the isomers, consistent with intrinsic reaction coordinate calculations of the isomer ground state potential energy surfaces at the density functional level of theory, and consequently, the involvement of these highly energetic species on chemically-relevant time scales needs to be taken into account. Monochlorocomplexes in methanol solutions promoted to the ligand-to-metal charge transfer (LMCT) excited state predominantly undergo internal conversion via back electron transfer, giving rise to vibrationally hot ground-state parent complexes. Copper-chloride homolitical bond dissociation yielding the solvated copper(I) and Cl- atom/solvent CT complexes constitutes a minor pathway. Insights into ligand substitution mechanisms were acquired by monitoring the recovery of monochloro complexes at the expense of two unexcited dichloro- and unsubstituted forms of Cu(II) complexes also present in the solution. Detailed description of ultrafast excited-state dynamics of CuCl 42- complexes in acetonitrile upon excitation into all possible Ligand Field (LF) excited states and two most intense LMCT transitions is reported. The LF states were found to be nonreactive with lifetimes remarkably longer than those

Ultrafast all-optical switching and error-free 10 Gbit/s wavelength conversion in hybrid InP-silicon on insulator nanocavities using surface quantum wells

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

Bazin, Alexandre; Monnier, Paul; Beaudoin, Grégoire

Ultrafast switching with low energies is demonstrated using InP photonic crystal nanocavities embedding InGaAs surface quantum wells heterogeneously integrated to a silicon on insulator waveguide circuitry. Thanks to the engineered enhancement of surface non radiative recombination of carriers, switching time is obtained to be as fast as 10 ps. These hybrid nanostructures are shown to be capable of achieving systems level performance by demonstrating error free wavelength conversion at 10 Gbit/s with 6 mW switching powers.

Reconstruction of instantaneous surface normal velocity of a vibrating structure using interpolated time-domain equivalent source method

NASA Astrophysics Data System (ADS)

Geng, Lin; Bi, Chuan-Xing; Xie, Feng; Zhang, Xiao-Zheng

2018-07-01

Interpolated time-domain equivalent source method is extended to reconstruct the instantaneous surface normal velocity of a vibrating structure by using the time-evolving particle velocity as the input, which provides a non-contact way to overall understand the instantaneous vibration behavior of the structure. In this method, the time-evolving particle velocity in the near field is first modeled by a set of equivalent sources positioned inside the vibrating structure, and then the integrals of equivalent source strengths are solved by an iterative solving process and are further used to calculate the instantaneous surface normal velocity. An experiment of a semi-cylindrical steel plate impacted by a steel ball is investigated to examine the ability of the extended method, where the time-evolving normal particle velocity and pressure on the hologram surface measured by a Microflown pressure-velocity probe are used as the inputs of the extended method and the method based on pressure measurements, respectively, and the instantaneous surface normal velocity of the plate measured by a laser Doppler vibrometry is used as the reference for comparison. The experimental results demonstrate that the extended method is a powerful tool to visualize the instantaneous surface normal velocity of a vibrating structure in both time and space domains and can obtain more accurate results than that of the method based on pressure measurements.

Monte Carlo wave packet study of negative ion mediated vibrationally inelastic scattering of NO from the metal surface

NASA Astrophysics Data System (ADS)

Li, Shenmin; Guo, Hua

2002-09-01

The scattering dynamics of vibrationally excited NO from a metal surface is investigated theoretically using a dissipative model that includes both the neutral and negative ion states. The Liouville-von Neumann equation is solved numerically by a Monte Carlo wave packet method, in which the wave packet is allowed to "jump" between the neutral and negative ion states in a stochastic fashion. It is shown that the temporary population of the negative ion state results in significant changes in vibrational dynamics, which eventually lead to vibrationally inelastic scattering of NO. Reasonable agreement with experiment is obtained with empirical potential energy surfaces. In particular, the experimentally observed facile multiquantum relaxation of the vibrationally highly excited NO is reproduced. The simulation also provides interesting insight into the scattering dynamics.

Effect of vibration on retention characteristics of screen acquisition systems. [for surface tension propellant acquisition

NASA Technical Reports Server (NTRS)

Tegart, J. R.; Aydelott, J. C.

1978-01-01

The design of surface tension propellant acquisition systems using fine-mesh screen must take into account all factors that influence the liquid pressure differentials within the system. One of those factors is spacecraft vibration. Analytical models to predict the effects of vibration have been developed. A test program to verify the analytical models and to allow a comparative evaluation of the parameters influencing the response to vibration was performed. Screen specimens were tested under conditions simulating the operation of an acquisition system, considering the effects of such parameters as screen orientation and configuration, screen support method, screen mesh, liquid flow and liquid properties. An analytical model, based on empirical coefficients, was most successful in predicting the effects of vibration.

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

PubMed Central

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

2017-01-01

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

Effects of tibialis anterior vibration on postural control when exposed to support surface translations.

PubMed

Temple, David R; Lee, Beom-Chan; Layne, Charles S

2016-03-01

The sensory re-weighting theory suggests unreliable inputs may be down-weighted to favor more reliable sensory information and thus maintain proper postural control. This study investigated the effects of tibialis anterior (TA) vibration on center of pressure (COP) motion in healthy individuals exposed to support surface translations to further explore the concept of sensory re-weighting. Twenty healthy young adults stood with eyes closed and arms across their chest while exposed to randomized blocks of five trials. Each trial lasted 8 s, with TA vibration either on or off. After 2 s, a sudden backward or forward translation occurred. Anterior-posterior (A/P) COP data were evaluated during the preparatory (first 2 s), perturbation (next 3 s), and recovery (last 3 s) phases to assess the effect of vibration on perturbation response features. The knowledge of an impending perturbation resulted in reduced anterior COP motion with TA vibration in the preparatory phase relative to the magnitude of anterior motion typically observed during TA vibration. During the perturbation phase, vibration did not influence COP motion. However, during the recovery phase vibration induced greater anterior COP motion than during trials without vibration. The fact that TA vibration produced differing effects on COP motion depending upon the phase of the perturbation response may suggest that the immediate context during which postural control is being regulated affects A/P COP responses to TA vibration. This indicates that proprioceptive information is likely continuously re-weighted according to the context in order to maintain effective postural control.

Structural coloration of metallic surfaces with micro/nano-structures induced by elliptical vibration texturing

NASA Astrophysics Data System (ADS)

Yang, Yang; Pan, Yayue; Guo, Ping

2017-04-01

Creating orderly periodic micro/nano-structures on metallic surfaces, or structural coloration, for control of surface apparent color and optical reflectivity has been an exciting research topic over the years. The direct applications of structural coloration include color marking, display devices, and invisibility cloak. This paper presents an efficient method to colorize metallic surfaces with periodic micro/nano-gratings using elliptical vibration texturing. When the tool vibration is coupled with a constant cutting velocity, controlled periodic ripples can be generated due to the overlapping tool trajectory. These periodic ripples with a wavelength near visible spectrum can act as micro-gratings to introduce iridescent colors. The proposed technique also provides a flexible method for color marking of metallic surfaces with arbitrary patterns and images by precise control of the spacing distance and orientation of induced micro/nano-ripples. Theoretical analysis and experimental results are given to demonstrate structural coloration of metals by a direct mechanical machining technique.

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

Engineering the vibrational coherence of vision into a synthetic molecular device.

PubMed

Gueye, Moussa; Manathunga, Madushanka; Agathangelou, Damianos; Orozco, Yoelvis; Paolino, Marco; Fusi, Stefania; Haacke, Stefan; Olivucci, Massimo; Léonard, Jérémie

2018-01-22

The light-induced double-bond isomerization of the visual pigment rhodopsin operates a molecular-level optomechanical energy transduction, which triggers a crucial protein structure change. In fact, rhodopsin isomerization occurs according to a unique, ultrafast mechanism that preserves mode-specific vibrational coherence all the way from the reactant excited state to the primary photoproduct ground state. The engineering of such an energy-funnelling function in synthetic compounds would pave the way towards biomimetic molecular machines capable of achieving optimum light-to-mechanical energy conversion. Here we use resonance and off-resonance vibrational coherence spectroscopy to demonstrate that a rhodopsin-like isomerization operates in a biomimetic molecular switch in solution. Furthermore, by using quantum chemical simulations, we show why the observed coherent nuclear motion critically depends on minor chemical modifications capable to induce specific geometric and electronic effects. This finding provides a strategy for engineering vibrationally coherent motions in other synthetic systems.

Determining the location of buried plastic water pipes from measurements of ground surface vibration

NASA Astrophysics Data System (ADS)

Muggleton, J. M.; Brennan, M. J.; Gao, Y.

2011-09-01

‘Mapping the Underworld' is a UK-based project, which aims to create a multi-sensor device that combines complementary technologies for remote buried utility service detection and location. One of the technologies to be incorporated in the device is low-frequency vibro-acoustics, and techniques for detecting buried infrastructure, in particular plastic water pipes, are being investigated. One of the proposed techniques involves excitation of the pipe at some known location with concurrent vibrational mapping of the ground surface in order to infer the location of the remainder of the pipe. In this paper, measurements made on a dedicated pipe rig are reported. Frequency response measurements relating vibrational velocity on the ground to the input excitation were acquired. Contour plots of the unwrapped phase revealed the location of the pipe to within 0.1-0.2 m. Magnitude contour plots revealed the excitation point and also the location of the pipe end. By examining the unwrapped phase gradients along a line above the pipe, it was possible to identify the wave-type within the pipe responsible for the ground surface vibration. Furthermore, changes in the ground surface phase speed computed using this method enabled the location of the end of the pipe to be confirmed.

Effects on Vibration and Surface Roughness in High Speed Micro End-Milling of Inconel 718 with Minimum Quantity Lubrication

NASA Astrophysics Data System (ADS)

Rahman, Mohamed Abd; Yeakub Ali, Mohammad; Saddam Khairuddin, Amir

2017-03-01

This paper presents the study on vibration and surface roughness of Inconel 718 workpiece produced by micro end-milling using Mikrotools Integrated Multi-Process machine tool DT-110 with control parameters; spindle speed (15000 rpm and 30000 rpm), feed rate (2 mm/min and 4 mm/min) and depth of cut (0.10 mm and 0.15mm). The vibration was measured using DYTRAN accelerometer instrument and the average surface roughness Ra was measured using Wyko NT1100. The analysis of variance (ANOVA) by using Design Expert software revealed that feed rate and depth of cut are the most significant factors on vibration meanwhile for average surface roughness, Ra, spindle speed is the most significant factor.

Ultrafast electron transport across nano gaps in nanowire circuits

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

Potma, Eric O.

In this Program we aim for a closer look at electron transfer through single molecules. To achieve this, we use ultrafast laser pulses to time stamp an electron tunneling event in a molecule that is connected between two metallic electrodes, while reading out the electron current. A key aspect of this project is the use of metallic substrates with plasmonic activity to efficiently manipulate the tunneling probability. The first Phase of this program is concerned with developing highly sensitive tools for the ultrafast optical manipulation of tethered molecules through the evanescent surface field of plasmonic substrates. The second Phase ofmore » the program aims to use these tools for exercising control over the electron tunneling probability.« less

Proton--H/sub 2/ scattering on an ab initio CI potential energy surface. I. Vibrational excitation at 10 eV

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

Schinke, R.; Dupuis, M.; Lester, W.A. Jr.

1980-04-01

A complete configuration interaction (CI) ground state surface for the H/sub 3//sup +/ system has been calculated using 5S and 3(P/sub x/,P/sub y/,P/sub x/) basis functions at each center. A total of 650 nuclear geometries has been considered which makes the new surface appropriate not only for scattering calculations, but also for the evaluation of the vibrational--rotational spectrum of the H/sub 3//sup +/ molecule. Significant deviations are found from the analytic Giese and Gentry potential used in many previous theoretical studies, especially for large and small nonequilibrium H--H separations which are important for vibrational excitation of the H/sub 2/ molecule.more » Vibrational--rotational excitation cross sections have been calculated in the rotational sudden approximation where the vibrational degree of freedom is treated exactly by solving seven vibrationally coupled radial equations. The use of the new surface leads to increased vibrational excitation compared to previous calculations utilizing the same scattering approximation and to excellent agreement at 10 eV with the angle-dependent measurements of Hermann, Schmidt, and Linder.« less

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO 3

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

Chen, F.; Zhu, Y.; Liu, S.

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO 3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. Thismore » effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.« less

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO 3

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

Chen, F.; Zhu, Y.; Liu, S.

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here in this paper we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO 3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent acrossmore » unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.« less

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO 3

DOE PAGES

Chen, F.; Zhu, Y.; Liu, S.; ...

2016-11-22

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here in this paper we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO 3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent acrossmore » unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.« less

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

DOE PAGES

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

2014-12-15

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

Hot electron dynamics at semiconductor surfaces: Implications for quantum dot photovoltaics

NASA Astrophysics Data System (ADS)

Tisdale, William A., III

. A TR-SHG study of these electronically-coupled quantum-dot films reveals temperature-activated cooling of hot charge carriers and coherent excitation of a previously-unidentified surface optical phonon. Finally, I report the first experimental observation of ultrafast electron transfer from the higher excited states of a colloidal quantum dot (PbSe) to delocalized conduction band states of a widely-used electron acceptor (TiO2). The electric field resulting from ultrafast (<50fs) separation of charge carriers across the PbSe/TiO2(110) interface excites coherent vibration of the TiO2 surface atoms, whose collective motions can be followed in real time.

Ultrafast dynamics of the lowest-lying neutral states in carbon dioxide

DOE PAGES

Wright, Travis W.; Champenois, Elio G.; Cryan, James P.; ...

2017-02-17

Here, we present a study of the ultrafast dissociation dynamics of the lowest-lying electronic excited states in CO 2 by using ultraviolet (UV) and extreme-ultraviolet (XUV) pulses from high-order harmonic generation. We observe two primary dissociation channels: a direct dissociation channel along the 1Π g electronically excited manifold, and a second channel which results from the mixing of electronic states. The direct dissociation channel is found to have a lifetime which is shorter than our experimental resolution, whereas the second channel has a significantly longer lifetime of nearly 200 fs. In this long-lived channel we observe a beating of themore » vibrational populations with a period of ~133 fs.« less

Laser-driven high-frequency vibrations of metal blister surface

NASA Astrophysics Data System (ADS)

Kononenko, T. V.; Sinyavsky, M. N.; Konov, V. I.; Sentis, M.

2013-09-01

Time-resolved interferometric microscopy was applied to investigate laser-induced blistering of a titanium film on a silica substrate. Ablation of the titanium/silica interface by single 0.7 ns pulses within a certain fluence range results in local exfoliation of the metal film from the substrate avoiding, however, complete film destruction. Time-dependent transformation of the metal surface profile was reconstructed from the interference patterns within 0-13 ns time delay range. Transverse annular waves with typical amplitude of one hundred of nanometers and estimated traveling speed of few kilometers per second were revealed on the blister surface. The wave occurrence was attributed to fast inhomogeneous bending of the film covering the expanding blister. The resultant high-frequency (˜1 GHz) vibrations of the metal surface provide intensive inertial forces when such metalized target is used for blister-based laser-induced forward transfer of nanopowders and organic molecules.

The Effect of Surface Wave Propagation on Neural Responses to Vibration in Primate Glabrous Skin

PubMed Central

Manfredi, Louise R.; Baker, Andrew T.; Elias, Damian O.; Dammann, John F.; Zielinski, Mark C.; Polashock, Vicky S.; Bensmaia, Sliman J.

2012-01-01

Because tactile perception relies on the response of large populations of receptors distributed across the skin, we seek to characterize how a mechanical deformation of the skin at one location affects the skin at another. To this end, we introduce a novel non-contact method to characterize the surface waves produced in the skin under a variety of stimulation conditions. Specifically, we deliver vibrations to the fingertip using a vibratory actuator and measure, using a laser Doppler vibrometer, the surface waves at different distances from the locus of stimulation. First, we show that a vibration applied to the fingertip travels at least the length of the finger and that the rate at which it decays is dependent on stimulus frequency. Furthermore, the resonant frequency of the skin matches the frequency at which a subpopulation of afferents, namely Pacinian afferents, is most sensitive. We show that this skin resonance can lead to a two-fold increase in the strength of the response of a simulated afferent population. Second, the rate at which vibrations propagate across the skin is dependent on the stimulus frequency and plateaus at 7 m/s. The resulting delay in neural activation across locations does not substantially blur the temporal patterning in simulated populations of afferents for frequencies less than 200 Hz, which has important implications about how vibratory frequency is encoded in the responses of somatosensory neurons. Third, we show that, despite the dependence of decay rate and propagation speed on frequency, the waveform of a complex vibration is well preserved as it travels across the skin. Our results suggest, then, that the propagation of surface waves promotes the encoding of spectrally complex vibrations as the entire neural population is exposed to essentially the same stimulus. We also discuss the implications of our results for biomechanical models of the skin. PMID:22348055

Temperature and chain length dependence of ultrafast vibrational dynamics of thiocyanate in alkylimidazolium ionic liquids: A random walk on a rugged energy landscape.

PubMed

Brinzer, Thomas; Garrett-Roe, Sean

2017-11-21

Ultrafast two-dimensional infrared spectroscopy of a thiocyanate vibrational probe (SCN - ) was used to investigate local dynamics in alkylimidazolium bis-[trifluoromethylsulfonyl]imide ionic liquids ([Im n,1 ][Tf 2 N], n = 2, 4, 6) at temperatures from 5 to 80 °C. The rate of frequency fluctuations reported by SCN - increases with increasing temperature and decreasing alkyl chain length. Temperature-dependent correlation times scale proportionally to temperature-dependent bulk viscosities of each ionic liquid studied. A multimode Brownian oscillator model demonstrates that very low frequency (<10 cm -1 ) modes primarily drive the observed spectral diffusion and that these modes broaden and blue shift on average with increasing temperature. An Arrhenius analysis shows activation barriers for local motions around the probe between 5.5 and 6.5 kcal/mol that are very similar to those for translational diffusion of ions. [Im 6,1 ][Tf 2 N] shows an unexpected decrease in activation energy compared to [Im 4,1 ][Tf 2 N] that may be related to mesoscopically ordered polar and nonpolar domains. A model of dynamics on a rugged potential energy landscape provides a unifying description of the observed Arrhenius behavior and the Brownian oscillator model of the low frequency modes.

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.

Single-electron pulses for ultrafast diffraction

PubMed Central

Aidelsburger, M.; Kirchner, F. O.; Krausz, F.; Baum, P.

2010-01-01

Visualization of atomic-scale structural motion by ultrafast electron diffraction and microscopy requires electron packets of shortest duration and highest coherence. We report on the generation and application of single-electron pulses for this purpose. Photoelectric emission from metal surfaces is studied with tunable ultraviolet pulses in the femtosecond regime. The bandwidth, efficiency, coherence, and electron pulse duration are investigated in dependence on excitation wavelength, intensity, and laser bandwidth. At photon energies close to the cathode’s work function, the electron pulse duration shortens significantly and approaches a threshold that is determined by interplay of the optical pulse width and the acceleration field. An optimized choice of laser wavelength and bandwidth results in sub-100-fs electron pulses. We demonstrate single-electron diffraction from polycrystalline diamond films and reveal the favorable influences of matched photon energies on the coherence volume of single-electron wave packets. We discuss the consequences of our findings for the physics of the photoelectric effect and for applications of single-electron pulses in ultrafast 4D imaging of structural dynamics. PMID:21041681

Recovering Intrinsic Fragmental Vibrations Using the Generalized Subsystem Vibrational Analysis.

PubMed

Tao, Yunwen; Tian, Chuan; Verma, Niraj; Zou, Wenli; Wang, Chao; Cremer, Dieter; Kraka, Elfi

2018-05-08

Normal vibrational modes are generally delocalized over the molecular system, which makes it difficult to assign certain vibrations to specific fragments or functional groups. We introduce a new approach, the Generalized Subsystem Vibrational Analysis (GSVA), to extract the intrinsic fragmental vibrations of any fragment/subsystem from the whole system via the evaluation of the corresponding effective Hessian matrix. The retention of the curvature information with regard to the potential energy surface for the effective Hessian matrix endows our approach with a concrete physical basis and enables the normal vibrational modes of different molecular systems to be legitimately comparable. Furthermore, the intrinsic fragmental vibrations act as a new link between the Konkoli-Cremer local vibrational modes and the normal vibrational modes.

Ultrafast Bessel beams: advanced tools for laser materials processing

NASA Astrophysics Data System (ADS)

Stoian, Razvan; Bhuyan, Manoj K.; Zhang, Guodong; Cheng, Guanghua; Meyer, Remy; Courvoisier, Francois

2018-05-01

Ultrafast Bessel beams demonstrate a significant capacity of structuring transparent materials with a high degree of accuracy and exceptional aspect ratio. The ability to localize energy on the nanometer scale (bypassing the 100-nm milestone) makes them ideal tools for advanced laser nanoscale processing on surfaces and in the bulk. This allows to generate and combine micron and nano-sized features into hybrid structures that show novel functionalities. Their high aspect ratio and the accurate location can equally drive an efficient material modification and processing strategy on large dimensions. We review, here, the main concepts of generating and using Bessel non-diffractive beams and their remarkable features, discuss general characteristics of their interaction with matter in ablation and material modification regimes, and advocate their use for obtaining hybrid micro and nanoscale structures in two and three dimensions (2D and 3D) performing complex functions. High-throughput applications are indicated. The example list ranges from surface nanostructuring and laser cutting to ultrafast laser welding and the fabrication of 3D photonic systems embedded in the volume.

Application of the wavelet packet transform to vibration signals for surface roughness monitoring in CNC turning operations

NASA Astrophysics Data System (ADS)

García Plaza, E.; Núñez López, P. J.

2018-01-01

The wavelet packet transform method decomposes a time signal into several independent time-frequency signals called packets. This enables the temporary location of transient events occurring during the monitoring of the cutting processes, which is advantageous in monitoring condition and fault diagnosis. This paper proposes the monitoring of surface roughness using a single low cost sensor that is easily implemented in numerical control machine tools in order to make on-line decisions on workpiece surface finish quality. Packet feature extraction in vibration signals was applied to correlate the sensor signals to measured surface roughness. For the successful application of the WPT method, mother wavelets, packet decomposition level, and appropriate packet selection methods should be considered, but are poorly understood aspects in the literature. In this novel contribution, forty mother wavelets, optimal decomposition level, and packet reduction methods were analysed, as well as identifying the effective frequency range providing the best packet feature extraction for monitoring surface finish. The results show that mother wavelet biorthogonal 4.4 in decomposition level L3 with the fusion of the orthogonal vibration components (ax + ay + az) were the best option in the vibration signal and surface roughness correlation. The best packets were found in the medium-high frequency DDA (6250-9375 Hz) and high frequency ADA (9375-12500 Hz) ranges, and the feed acceleration component ay was the primary source of information. The packet reduction methods forfeited packets with relevant features to the signal, leading to poor results for the prediction of surface roughness. WPT is a robust vibration signal processing method for the monitoring of surface roughness using a single sensor without other information sources, satisfactory results were obtained in comparison to other processing methods with a low computational cost.

Vibrational Studies of Adsorbate-Induced Reconstruction on Molybdenum Surfaces.

NASA Astrophysics Data System (ADS)

Lopinski, Gregory Peter

as well as the form of the observed coverage dependence differ from the predictions of the traditional charge transfer model of alkali adsorption. The relevance of the vibrational results to the Na-induced structural changes observed on this surface are also discussed. Na adsorption has been found to dramatically alter the interaction of oxygen with this surface, due to the presence of a strong attractive interaction between Na and O that forces O atoms to occupy a different binding site than on a clean surface.

Surface modified CF x cathode material for ultrafast discharge and high energy density

DOE PAGES

Dai, Yang; Zhu, Yimei; Cai, Sendan; ...

2014-11-10

Li/CF x primary possesses the highest energy density of 2180 W h kg⁻¹ among all primary lithium batteries. However, a key limitation for the utility of this type of battery is in its poor rate capability because the cathode material, CF x, is an intrinsically poor electronic conductor. Here, we report on our development of a controlled process of surface de-fluorination under mild hydrothermal conditions to modify the highly fluorinated CF x. The modified CF x, consisting of an in situ generated shell component of F-graphene layers, possesses good electronic conductivity and removes the transporting barrier for lithium ions, yieldingmore » a high-capacity performance and an excellent rate-capability. Indeed, a capacity of 500 mA h g⁻¹ and a maximum power density of 44 800 W kg⁻¹ can be realized at the ultrafast rate of 30 C (24 A g⁻¹), which is over one order of magnitude higher than that of the state-of-the-art primary lithium-ion batteries.« less

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.

Long-Range Vibrational Dynamics Are Directed by Watson-Crick Base Pairing in Duplex DNA.

PubMed

Hithell, Gordon; Shaw, Daniel J; Donaldson, Paul M; Greetham, Gregory M; Towrie, Michael; Burley, Glenn A; Parker, Anthony W; Hunt, Neil T

2016-05-05

Ultrafast two-dimensional infrared (2D-IR) spectroscopy of a 15-mer A-T DNA duplex in solution has revealed structure-dependent vibrational coupling and energy transfer processes linking bases with the sugar-phosphate backbone. Duplex melting induces significant changes in the positions of off-diagonal peaks linking carbonyl and ring-stretching vibrational modes of the adenine and thymine bases with vibrations of the phosphate group and phosphodiester linkage. These indicate that Watson-Crick hydrogen bonding and helix formation lead to a unique vibrational coupling arrangement of base vibrational modes with those of the phosphate unit. On the basis of observations from time-resolved 2D-IR data, we conclude that rapid energy transfer processes occur between base and backbone, mediated by additional modes located on the deoxyribose moiety within the same nucleotide. These relaxation dynamics are insensitive to duplex melting, showing that efficient intramolecular energy relaxation to the solvent via the phosphate groups is the key to excess energy dissipation in both single- and double-stranded DNA.

Ultra-fast relaxation, decoherence, and localization of photoexcited states in π-conjugated polymers

NASA Astrophysics Data System (ADS)

Mannouch, Jonathan R.; Barford, William; Al-Assam, Sarah

2018-01-01

The exciton relaxation dynamics of photoexcited electronic states in poly(p-phenylenevinylene) are theoretically investigated within a coarse-grained model, in which both the exciton and nuclear degrees of freedom are treated quantum mechanically. The Frenkel-Holstein Hamiltonian is used to describe the strong exciton-phonon coupling present in the system, while external damping of the internal nuclear degrees of freedom is accounted for by a Lindblad master equation. Numerically, the dynamics are computed using the time evolving block decimation and quantum jump trajectory techniques. The values of the model parameters physically relevant to polymer systems naturally lead to a separation of time scales, with the ultra-fast dynamics corresponding to energy transfer from the exciton to the internal phonon modes (i.e., the C-C bond oscillations), while the longer time dynamics correspond to damping of these phonon modes by the external dissipation. Associated with these time scales, we investigate the following processes that are indicative of the system relaxing onto the emissive chromophores of the polymer: (1) Exciton-polaron formation occurs on an ultra-fast time scale, with the associated exciton-phonon correlations present within half a vibrational time period of the C-C bond oscillations. (2) Exciton decoherence is driven by the decay in the vibrational overlaps associated with exciton-polaron formation, occurring on the same time scale. (3) Exciton density localization is driven by the external dissipation, arising from "wavefunction collapse" occurring as a result of the system-environment interactions. Finally, we show how fluorescence anisotropy measurements can be used to investigate the exciton decoherence process during the relaxation dynamics.

Carbonyl iron powder surface modification of magnetorheological elastomers for vibration absorbing application

NASA Astrophysics Data System (ADS)

Chen, Dong; Yu, Miao; Zhu, Mi; Qi, Song; Fu, Jie

2016-11-01

With excellent characteristic of magnetic-control stiffness, magnetorheological elastomer (MRE) is well suited as a spring element of vibration absorber. To improve the vibration attenuation performance of MRE vibration absorbers, this paper expects to improve the mechanical strength and reduce the loss factor of MRE by interface modification. The surface of carbonyl iron powder (CIP) was modified with silica coating by a simple and convenient approach. Several MRE samples, with different proportions of modified CIPs were fabricated under a constant magnetic field. The morphology and composition of modified CIP were characterized by scanning electron microscope and Fourier transform infrared spectra. The results indicated that the modified CIPs were coated with uniform and continuous silica, which can make a better combination between particle and matrix. The tensile strength, magnetorheological properties and the damping properties of the MRE samples were tested by material testing machine and rheometer. The experimental results demonstrated that the loss factor of the MRE which incorporated with modified CIPs decreased markedly, and the tensile strength of such material has been much improved, at the same time this kind of MRE kept high MR effect. It is expected that this MRE material will meet the requirements of vibration absorber.

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.

The (FHCl)- molecular anion - Structural aspects, global surface, and vibrational eigenspectrum

NASA Technical Reports Server (NTRS)

Klepeis, Neil E.; East, Allan L. L.; Csaszar, Attila G.; Allen, Wesley D.; Lee, Timothy J.; Schwenke, David W.

1993-01-01

State of the art ab initio electronic structure methods have been used to investigate the (FHCl)- molecular anion. It is proposed that the geometric structure and binding energies of the complex are r(e)(H-F) = 0.963 +/- 0.003 A, R(e)(H-Cl) = 1.925 +/- 0.015 A, and D0(HF + Cl(-)) = 21.8 +/- 0.4 kcal/mol. A Morokuma decomposition of the ion-molecular bonding give the following electrostatic, polarization, exchange repulsion, dispersion, and charge-transfer plus higher-order mixing components of the vibrationless complexation energy: -27.3, -5.2, +18.3, -4.5, and -5.0 kcal/mol, respectively. A couples cluster single and doubles global surface is constructed from 208 and 228 energy points for linear and bent configurations, respectively, these being fit to rms errors of only 3.9 and 9.3/cm, respectively, below 8000/cm. Converged J = 0 and J = 1 variational eigenstates of the (FHCl)- surface to near the HF + Cl(-) dissociation threshold are determined. The fundamental vibrational frequencies are found to be nu1 = 247/cm, nu2 = 876/cm, and nu3 = 2884/cm. The complete vibrational eigenspectrum is analyzed.

Ablation experiment and threshold calculation of titanium alloy irradiated by ultra-fast pulse laser

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

Zheng, Buxiang; Jiang, Gedong; Wang, Wenjun, E-mail: wenjunwang@mail.xjtu.edu.cn

The interaction between an ultra-fast pulse laser and a material's surface has become a research hotspot in recent years. Micromachining of titanium alloy with an ultra-fast pulse laser is a very important research direction, and it has very important theoretical significance and application value in investigating the ablation threshold of titanium alloy irradiated by ultra-fast pulse lasers. Irradiated by a picosecond pulse laser with wavelengths of 1064 nm and 532 nm, the surface morphology and feature sizes, including ablation crater width (i.e. diameter), ablation depth, ablation area, ablation volume, single pulse ablation rate, and so forth, of the titanium alloymore » were studied, and their ablation distributions were obtained. The experimental results show that titanium alloy irradiated by a picosecond pulse infrared laser with a 1064 nm wavelength has better ablation morphology than that of the green picosecond pulse laser with a 532 nm wavelength. The feature sizes are approximately linearly dependent on the laser pulse energy density at low energy density and the monotonic increase in laser pulse energy density. With the increase in energy density, the ablation feature sizes are increased. The rate of increase in the feature sizes slows down gradually once the energy density reaches a certain value, and gradually saturated trends occur at a relatively high energy density. Based on the linear relation between the laser pulse energy density and the crater area of the titanium alloy surface, and the Gaussian distribution of the laser intensity on the cross section, the ablation threshold of titanium alloy irradiated by an ultra-fast pulse laser was calculated to be about 0.109 J/cm{sup 2}.« less

Surface vibrational relaxation of N2 studied by CO2 titration with time-resolved quantum cascade laser absorption spectroscopy

NASA Astrophysics Data System (ADS)

Marinov, D.; Lopatik, D.; Guaitella, O.; Hübner, M.; Ionikh, Y.; Röpcke, J.; Rousseau, A.

2012-05-01

A new method for determination of the wall de-excitation probability \\gamma _{N_2 } of vibrationally excited N2 on different surfaces exposed to low-pressure plasmas has been developed. A short dc discharge pulse of only a few milliseconds was applied to a mixture containing 0.05-1% of CO2 in N2 at a pressure of 133 Pa. Due to a nearly resonant fast vibrational transfer between N2(v) and the asymmetric ν3 mode of CO2 the vibrational excitation of these titrating molecules is an image of the degree of vibrational excitation of N2. In the afterglow, the vibrational relaxation of CO2 was monitored in situ using quantum cascade laser absorption spectroscopy. The experimental results were interpreted in terms of a numerical model of non-equilibrium vibrational kinetics in CO2-N2 mixtures. Heterogeneous relaxation was the main quenching process of N2(v) under the conditions of this study, which allowed determination of the value of \\gamma _{N_2 } from the best agreement between the experiment and the model. The new method is suitable for \\gamma _{N_2 } determination in a single plasma pulse with the discharge tube surface pretreated by a low-pressure plasma. The relaxation probability of the first vibrational level of nitrogen γ1 = (1.1 ± 0.15) × 10-3 found for Pyrex and silica is in reasonable agreement with the literature data. Using the new technique the N2(v = 1) quenching probability was measured on TiO2 surface, γ1 = (9 ± 1) × 10-3. A linear enhancement of the N2(v) wall deactivation probability with an increase in the admixture of CO2 was observed for all studied materials. In order to explain this effect, a vibrational energy transfer mechanism between N2(v) and adsorbed CO2 is proposed.

Evidence for a vibrational phase-dependent isotope effect on the photochemistry of vision.

PubMed

Schnedermann, C; Yang, X; Liebel, M; Spillane, K M; Lugtenburg, J; Fernández, I; Valentini, A; Schapiro, I; Olivucci, M; Kukura, P; Mathies, R A

2018-04-01

Vibronic coupling is key to efficient energy flow in molecular systems and a critical component of most mechanisms invoking quantum effects in biological processes. Despite increasing evidence for coherent coupling of electronic states being mediated by vibrational motion, it is not clear how and to what degree properties associated with vibrational coherence such as phase and coupling of atomic motion can impact the efficiency of light-induced processes under natural, incoherent illumination. Here, we show that deuteration of the H 11 -C 11 =C 12 -H 12 double-bond of the 11-cis retinal chromophore in the visual pigment rhodopsin significantly and unexpectedly alters the photoisomerization yield while inducing smaller changes in the ultrafast isomerization dynamics assignable to known isotope effects. Combination of these results with non-adiabatic molecular dynamics simulations reveals a vibrational phase-dependent isotope effect that we suggest is an intrinsic attribute of vibronically coherent photochemical processes.

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

PubMed

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

2017-08-21

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

Ultrafast time-resolved pump-probe spectroscopy of PYP by a sub-8 fs pulse laser at 400 nm.

PubMed

Liu, Jun; Yabushita, Atsushi; Taniguchi, Seiji; Chosrowjan, Haik; Imamoto, Yasushi; Sueda, Keiichi; Miyanaga, Noriaki; Kobayashi, Takayoshi

2013-05-02

Impulsive excitation of molecular vibration is known to induce wave packets in both the ground state and excited state. Here, the ultrafast dynamics of PYP was studied by pump-probe spectroscopy using a sub-8 fs pulse laser at 400 nm. The broadband spectrum of the UV pulse allowed us to detect the pump-probe signal covering 360-440 nm. The dependence of the vibrational phase of the vibrational mode around 1155 cm(-1) on the probe photon energy was observed for the first time to our knowledge. The vibrational mode coupled to the electronic transition observed in the probe spectral ranges of 2.95-3.05 and 3.15-3.35 eV was attributed to the wave packets in the ground state and the excited state, respectively. The frequencies in the ground state and excited state were determined to be 1155 ± 1 and 1149 ± 1 cm(-1), respectively. The frequency difference is due to change after photoexcitation. This means a reduction of the bond strength associated with π-π* excitation, which is related to the molecular structure change associated with the primary isomerization process in the photocycle in PYP. Real-time vibrational modes at low frequency around 138, 179, 203, 260, and 317 cm(-1) were also observed and compared with the Raman spectrum for the assignment of the vibrational wave packet.

A new composite adaptive controller featuring the neural network and prescribed sliding surface with application to vibration control

NASA Astrophysics Data System (ADS)

Phu, Do Xuan; Huy, Ta Duc; Mien, Van; Choi, Seung-Bok

2018-07-01

This work proposes a novel composite adaptive controller based on the prescribed performance of the sliding surface and applies it to vibration control of a semi-active vehicle seat suspension system subjected to severe external disturbances. As a first step, the online fast interval type 2 fuzzy neural network system is adopted to establish a model and two sliding surfaces are used; conventional surface and prescribed surface. Then, an equivalent control is determined by assuming the derivative of the prescribed surface is zero, followed by the design of a controller which can guarantee both stability and robustness. Then, two controllers are combined and integrated with adaptation laws using the projection algorithm. The effectiveness of the proposed composite controller is validated through both simulation and experiment by undertaking vibration control of a semi-active seat suspension system equipped with a magneto-rheological (MR) damper. It is shown from both simulation and experimental realization that excellent vibration control performances are achieved with a small tracking error between the proposed and prescribed objectives. In addition, the control superiority of the proposed controller to conventional sliding mode controller featuring one sliding surface and proportional-integral-derivative (PID) controllers are demonstrated through a comparative work.

The fundamental role of quantized vibrations in coherent light harvesting by cryptophyte algae

NASA Astrophysics Data System (ADS)

Kolli, Avinash; O'Reilly, Edward J.; Scholes, Gregory D.; Olaya-Castro, Alexandra

2012-11-01

The influence of fast vibrations on energy transfer and conversion in natural molecular aggregates is an issue of central interest. This article shows the important role of high-energy quantized vibrations and their non-equilibrium dynamics for energy transfer in photosynthetic systems with highly localized excitonic states. We consider the cryptophyte antennae protein phycoerythrin 545 and show that coupling to quantized vibrations, which are quasi-resonant with excitonic transitions is fundamental for biological function as it generates non-cascaded transport with rapid and wider spatial distribution of excitation energy. Our work also indicates that the non-equilibrium dynamics of such vibrations can manifest itself in ultrafast beating of both excitonic populations and coherences at room temperature, with time scales in agreement with those reported in experiments. Moreover, we show that mechanisms supporting coherent excitonic dynamics assist coupling to selected modes that channel energy to preferential sites in the complex. We therefore argue that, in the presence of strong coupling between electronic excitations and quantized vibrations, a concrete and important advantage of quantum coherent dynamics is precisely to tune resonances that promote fast and effective energy distribution.

Vibrational energy distribution in aniline scattered from surfaces covered with organized organic monolayers

NASA Astrophysics Data System (ADS)

Paz, Y.; Naaman, R.

1990-08-01

Energy distribution in aniline molecules scattered from organized organic monolayers was investigated using a resonance-enhanced two-photon ionization technique. Two type of monolayers were used, one exposing a floppy unsubstituted aliphatic chain (OTS, n-octadecyltrichlorosilane), and the second having a perfluorinated tail (PFDA, perfluorodecanoic acid). The dependence of the internal and translational energy of the scattered aniline is monitored as a function of collision energy and surface properties. The data reveal an unusually high propensity for excitation of the NH 2 inversion mode in aniline. Vibrationally excited molecules are scattered with a narrower time-of-flight (TOF) distribution than those in the ground vibrational state.

Raman spectroscopy: Watching a molecule breathe

NASA Astrophysics Data System (ADS)

Piatkowski, Lukasz; Hugall, James T.; van Hulst, Niek F.

2014-08-01

Marrying the single-molecule detection ability of surface-enhanced Raman scattering with the extreme time resolution of ultrafast coherent spectroscopy enables the vibrations of a single molecule to be observed.

Soliton microdynamics of the generation of new-type nonlinear surface vibrations, dissociation, and surfing diffusion in diatomic crystals of the uranium nitride type

NASA Astrophysics Data System (ADS)

Dubovsky, O. A.; Semenov, V. A.; Orlov, A. V.; Sudarev, V. V.

2014-09-01

The microdynamics of large-amplitude nonlinear vibrations of uranium nitride diatomic lattices has been investigated using the computer simulation and neutron scattering methods at temperatures T = 600-2500°C near the thresholds of the dissociation and destruction of the reactor fuel materials. It has been found using the computer simulation that, in the spectral gap between the frequency bands of acoustic and optical phonons in crystals with an open surface, there are resonances of new-type harmonic surface vibrations and a gap-filling band of their genetic successors, i.e., nonlinear surface vibrations. Experimental measurements of the slow neutron scattering spectra of uranium nitride on the DIN-2PI neutron spectrometer have revealed resonances and bands of these surface vibrations in the spectral gap, as well as higher optical vibration overtones. It has been shown that the solitons and bisolitons initiate the formation and collapse of dynamic pores with the generation of surface vibrations at the boundaries of the cavities, evaporation of atoms and atomic clusters, formation of cracks, and destruction of the material. It has been demonstrated that the mass transfer of nitrogen in cracks and along grain boundaries can occur through the revealed microdynamics mechanism of the surfing diffusion of light nitrogen atoms at large-amplitude soliton waves propagating in the stabilizing sublattice of heavy uranium atoms and in the nitrogen sublattice.

Ordered water structure at hydrophobic graphite interfaces observed by 4D, ultrafast electron crystallography

PubMed Central

Yang, Ding-Shyue; Zewail, Ahmed H.

2009-01-01

Interfacial water has unique properties in various functions. Here, using 4-dimensional (4D), ultrafast electron crystallography with atomic-scale spatial and temporal resolution, we report study of structure and dynamics of interfacial water assembly on a hydrophobic surface. Structurally, vertically stacked bilayers on highly oriented pyrolytic graphite surface were determined to be ordered, contrary to the expectation that the strong hydrogen bonding of water on hydrophobic surfaces would dominate with suppressed interfacial order. Because of its terrace morphology, graphite plays the role of a template. The dynamics is also surprising. After the excitation of graphite by an ultrafast infrared pulse, the interfacial ice structure undergoes nonequilibrium “phase transformation” identified in the hydrogen-bond network through the observation of structural isosbestic point. We provide the time scales involved, the nature of ice-graphite structural dynamics, and relevance to properties related to confined water. PMID:19246378

Time-resolved vibrational spectroscopy

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

Tokmakoff, Andrei; Champion, Paul; Heilweil, Edwin J.

2009-05-14

This document contains the Proceedings from the 14th International Conference on Time-Resolved Vibrational Spectroscopy, which was held in Meredith, NH from May 9-14, 2009. The study of molecular dynamics in chemical reaction and biological processes using time-resolved spectroscopy plays an important role in our understanding of energy conversion, storage, and utilization problems. Fundamental studies of chemical reactivity, molecular rearrangements, and charge transport are broadly supported by the DOE's Office of Science because of their role in the development of alternative energy sources, the understanding of biological energy conversion processes, the efficient utilization of existing energy resources, and the mitigation ofmore » reactive intermediates in radiation chemistry. In addition, time-resolved spectroscopy is central to all fiveof DOE's grand challenges for fundamental energy science. The Time-Resolved Vibrational Spectroscopy conference is organized biennially to bring the leaders in this field from around the globe together with young scientists to discuss the most recent scientific and technological advances. The latest technology in ultrafast infrared, Raman, and terahertz spectroscopy and the scientific advances that these methods enable were covered. Particular emphasis was placed on new experimental methods used to probe molecular dynamics in liquids, solids, interfaces, nanostructured materials, and biomolecules.« less

Harmonium: An Ultrafast Vacuum Ultraviolet Facility.

PubMed

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

2017-05-31

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

Ultrafast ultrasound localization microscopy for deep super-resolution vascular imaging

NASA Astrophysics Data System (ADS)

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

2015-11-01

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

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

PubMed

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

2015-11-26

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

Vibrational energy transfer dynamics in ruthenium polypyridine transition metal complexes.

PubMed

Fedoseeva, Marina; Delor, Milan; Parker, Simon C; Sazanovich, Igor V; Towrie, Michael; Parker, Anthony W; Weinstein, Julia A

2015-01-21

Understanding the dynamics of the initial stages of vibrational energy transfer in transition metal complexes is a challenging fundamental question which is also of crucial importance for many applications, such as improving the performance of solar devices or photocatalysis. The present study investigates vibrational energy transport in the ground and the electronic excited state of Ru(4,4'-(COOEt)2-2,2-bpy)2(NCS)2, a close relative of the efficient "N3" dye used in dye-sensitized solar cells. Using the emerging technique of ultrafast two-dimensional infrared spectroscopy, we show that, similarly to other transition-metal complexes, the central Ru heavy atom acts as a "bottleneck" making the energy transfer from small ligands with high energy vibrational stretching frequencies less favorable and thereby affecting the efficiency of vibrational energy flow in the complex. Comparison of the vibrational relaxation times in the electronic ground and excited state of Ru(4,4'-(COOEt)2-2,2-bpy)2(NCS)2 shows that it is dramatically faster in the latter. We propose to explain this observation by the intramolecular electrostatic interactions between the thiocyanate group and partially oxidised Ru metal center, which increase the degree of vibrational coupling between CN and Ru-N modes in the excited state thus reducing structural and thermodynamic barriers that slow down vibrational relaxation and energy transport in the electronic ground state. As a very similar behavior was earlier observed in another transition-metal complex, Re(4,4'-(COOEt)2-2,2'-bpy)(CO)3Cl, we suggest that this effect in vibrational energy dynamics might be common for transition-metal complexes with heavy central atoms.

Effects of surface topography and vibrations on wetting: Superhydrophobicity, icephobicity and corrosion resistance

NASA Astrophysics Data System (ADS)

Ramachandran, Rahul

Concrete and metallic materials are widely used in construction and water industry. The interaction of both these materials with water and ice (or snow) produces undesirable results and is therefore of interest. Water that gets absorbed into the pores of dry concrete expands on freezing and can lead to crack formation. Also, the ice accretion on concrete surfaces such as roadways can have disastrous consequence. Metallic components used in the water industry undergo corrosion due to contact with aqueous corrosive solutions. Therefore, it is desirable to make concrete water/ice-repellent, and to make metallic surfaces corrosion-resistant. Recent advances in micro/nanotechnology have made it possible to design functional micro/nanostructured surfaces with micro/nanotopography providing low adhesion. Some examples of such surfaces are superhydrophobic surfaces, which are extremely water repellent, and icephobic surfaces, which have low ice adhesion, repel incoming water droplets before freezing, or delay ice nucleation. This dissertation investigates the effects of surface micro/nanotopography and small amplitude fast vibrations on the wetting and adhesion of concrete with the goal of producing hydrophobic and icephobic concrete, and on the wetting of metallic surfaces to prevent corrosion. The relationship between surface micro/nanotopography and small fast vibrations is established using the method of separation of motions. Both these small scale effects can be substituted by an effective force or energy. The structure-property relationships in materials and surfaces are established. Both vibrations as well as surface micro/nanopatterns can affect wetting properties such as contact angle and surface free energy. Hydrophobic engineered cementitious composite samples are produced by controlling their surface topography and surface free energy. The surface topography is controlled by varying the concrete mixture composition. The surface free energy of concrete is

Analysis of the Effects of Surface Pitting and Wear on the Vibrations of a Gear Transmission System

NASA Technical Reports Server (NTRS)

Choy, F. K.; Polyshchuk, V.; Zakrajsek, J. J.; Handschuh, R. F.; Townsend, D. P.

1994-01-01

A comprehensive procedure to simulate and analyze the vibrations in a gear transmission system with surface pitting, 'wear' and partial tooth fracture of the gear teeth is presented. An analytical model was developed where the effects of surface pitting and wear of the gear tooth were simulated by phase and magnitude changes in the gear mesh stiffness. Changes in the gear mesh stiffness were incorporated into each gear-shaft model during the global dynamic simulation of the system. The overall dynamics of the system were evaluated by solving for the transient dynamics of each shaft system simultaneously with the vibration of the gearbox structure. In order to reduce the number of degrees-of-freedom in the system, a modal synthesis procedure was used in the global transient dynamic analysis of the overall transmission system. An FFT procedure was used to transform the averaged time signal into the frequency domain for signature analysis. In addition, the Wigner-Ville distribution was also introduced to examine the gear vibration in the joint time frequency domain for vibration pattern recognition. Experimental results obtained from a gear fatigue test rig at NASA Lewis Research Center were used to evaluate the analytical model.

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.

Ultrafast and nanoscale diodes

NASA Astrophysics Data System (ADS)

Zhang, Peng; Lau, Y. Y.

2016-10-01

Charge carrier transport across interfaces of dissimilar materials (including vacuum) is the essence of all electronic devices. Ultrafast charge transport across a nanometre length scale is of fundamental importance in the miniaturization of vacuum and plasma electronics. With the combination of recent advances in electronics, photonics and nanotechnology, these miniature devices may integrate with solid-state platforms, achieving superior performance. This paper reviews recent modelling efforts on quantum tunnelling, ultrafast electron emission and transport, and electrical contact resistance. Unsolved problems and challenges in these areas are addressed.

Large lateral photovoltaic effect with ultrafast relaxation time in SnSe/Si junction

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

Wang, Xianjie; Zhao, Xiaofeng; Hu, Chang

In this paper, we report a large lateral photovoltaic effect (LPE) with ultrafast relaxation time in SnSe/p-Si junctions. The LPE shows a linear dependence on the position of the laser spot, and the position sensitivity is as high as 250 mV mm{sup −1}. The optical response time and the relaxation time of the LPE are about 100 ns and 2 μs, respectively. The current-voltage curve on the surface of the SnSe film indicates the formation of an inversion layer at the SnSe/p-Si interface. Our results clearly suggest that most of the excited-electrons diffuse laterally in the inversion layer at the SnSe/p-Si interface, whichmore » results in a large LPE with ultrafast relaxation time. The high positional sensitivity and ultrafast relaxation time of the LPE make the SnSe/p-Si junction a promising candidate for a wide range of optoelectronic applications.« less

Potential energy surface and vibrational band origins of the triatomic lithium cation

NASA Astrophysics Data System (ADS)

Searles, Debra J.; Dunne, Simon J.; von Nagy-Felsobuki, Ellak I.

The 104 point CISD Li +3 potential energy surface and its analytical representation is reported. The calculations predict the minimum energy geometry to be an equilateral triangle of side RLiLi = 3.0 Å and of energy - 22.20506 E h. A fifth-order Morse—Dunham type analytical force field is used in the Carney—Porter normal co-ordinate vibrational Hamiltonian, the corresponding eigenvalue problem being solved variationally using a 560 configurational finite-element basis set. The predicted assignment of the vibrational band origins is in accord with that reported for H +3. Moreover, for 6Li +3 and 7Li +3 the lowest i.r. accessible band origin is the overlineν0,1,±1 predicted to be at 243.6 and 226.0 cm -1 respectively.

The effect of ultrafast fiber laser application on the bond strength of resin cement to titanium.

PubMed

Ates, Sabit Melih; Korkmaz, Fatih Mehmet; Caglar, Ipek Satıroglu; Duymus, Zeynep Yeşil; Turgut, Sedanur; Bagis, Elif Arslan

2017-07-01

The purpose of this study was to investigate the effect of ultrafast fiber laser treatment on the bond strength between titanium and resin cement. A total of 60 pure titanium discs (15 mm × 2 mm) were divided into six test groups (n = 10) according to the surface treatment used: group (1) control, machining; group (2) grinding with a diamond bur; group (3) ultrafast fiber laser application; group (4) resorbable blast media (RBM) application; group (5) electro-erosion with copper; and group (6) sandblasting. After surface treatments, resin cements were applied to the treated titanium surfaces. Shear bond strength testing of the samples was performed with a universal testing machine after storing in distilled water at 37 °C for 24 h. One-way ANOVA and Tukey's HSD post hoc test were used to analyse the data (P < 0.05). The highest bond strength values were observed in the laser application group, while the lowest values were observed in the grinding group. Sandblasting and laser application resulted in significantly higher bond strengths than control treatment (P < 0.05). Ultrafast fiber laser treatment and sandblasting may improve the bond strength between resin cement and titanium.

Ab Initio Potential Energy Surfaces and the Calculation of Accurate Vibrational Frequencies

NASA Technical Reports Server (NTRS)

Lee, Timothy J.; Dateo, Christopher E.; Martin, Jan M. L.; Taylor, Peter R.; Langhoff, Stephen R. (Technical Monitor)

1995-01-01

Due to advances in quantum mechanical methods over the last few years, it is now possible to determine ab initio potential energy surfaces in which fundamental vibrational frequencies are accurate to within plus or minus 8 cm(exp -1) on average, and molecular bond distances are accurate to within plus or minus 0.001-0.003 Angstroms, depending on the nature of the bond. That is, the potential energy surfaces have not been scaled or empirically adjusted in any way, showing that theoretical methods have progressed to the point of being useful in analyzing spectra that are not from a tightly controlled laboratory environment, such as vibrational spectra from the interstellar medium. Some recent examples demonstrating this accuracy will be presented and discussed. These include the HNO, CH4, C2H4, and ClCN molecules. The HNO molecule is interesting due to the very large H-N anharmonicity, while ClCN has a very large Fermi resonance. The ab initio studies for the CH4 and C2H4 molecules present the first accurate full quartic force fields of any kind (i.e., whether theoretical or empirical) for a five-atom and six-atom system, respectively.

State-Resolved Metal Nanoparticle Dynamics Viewed through the Combined Lenses of Ultrafast and Magneto-optical Spectroscopies.

PubMed

Zhao, Tian; Herbert, Patrick J; Zheng, Hongjun; Knappenberger, Kenneth L

2018-06-19

Electronic carrier dynamics play pivotal roles in the functional properties of nanomaterials. For colloidal metals, the mechanisms and influences of these dynamics are structure dependent. The coherent carrier dynamics of collective plasmon modes for nanoparticles (approximately 2 nm and larger) determine optical amplification factors that are important to applied spectroscopy techniques. In the nanocluster domain (sub-2 nm), carrier coupling to vibrational modes affects photoluminescence yields. The performance of photocatalytic materials featuring both nanoparticles and nanoclusters also depends on the relaxation dynamics of nonequilibrium charge carriers. The challenges for developing comprehensive descriptions of carrier dynamics spanning both domains are multifold. Plasmon coherences are short-lived, persisting for only tens of femtoseconds. Nanoclusters exhibit discrete carrier dynamics that can persist for microseconds in some cases. On this time scale, many state-dependent processes, including vibrational relaxation, charge transfer, and spin conversion, affect carrier dynamics in ways that are nonscalable but, rather, structure specific. Hence, state-resolved spectroscopy methods are needed for understanding carrier dynamics in the nanocluster domain. Based on these considerations, a detailed understanding of structure-dependent carrier dynamics across length scales requires an appropriate combination of spectroscopic methods. Plasmon mode-specific dynamics can be obtained through ultrafast correlated light and electron microscopy (UCLEM), which pairs interferometric nonlinear optical (INLO) with electron imaging methods. INLO yields nanostructure spectral resonance responses, which capture the system's homogeneous line width and coherence dynamics. State-resolved nanocluster dynamics can be obtained by pairing ultrafast with magnetic-optical spectroscopy methods. In particular, variable-temperature variable-field (VTVH) spectroscopies allow quantification

Reduction of the coupling vibration between the bending vibrators of the frequency-change-type two-axis acceleration sensor

NASA Astrophysics Data System (ADS)

Sugawara, Sumio; Sasaki, Yoshifumi; Kudo, Subaru

2018-07-01

The frequency-change-type two-axis acceleration sensor uses a cross-type vibrator consisting of four bending vibrators. When coupling vibration exists between these four bending vibrators, the resonance frequency of each vibrator cannot be adjusted independently. In this study, methods of reducing the coupling vibration were investigated by finite-element analysis. A method of adjusting the length of the short arm of each vibrator was proposed for reducing the vibration. When piezoelectric ceramics were bonded to the single-sided surface of the vibrator, the method was not sufficient. Thus, the ceramics with the same dimensions were bonded to double-sided surfaces. As a result, a marked reduction was obtained in this case. Also, the linearity of the sensor characteristics was significantly improved in a small acceleration range. Accordingly, it was clarified that considering the symmetry along the thickness direction of the vibrator is very important.

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.

Staggered Multiple-PRF Ultrafast Color Doppler.

PubMed

Posada, Daniel; Poree, Jonathan; Pellissier, Arnaud; Chayer, Boris; Tournoux, Francois; Cloutier, Guy; Garcia, Damien

2016-06-01

Color Doppler imaging is an established pulsed ultrasound technique to visualize blood flow non-invasively. High-frame-rate (ultrafast) color Doppler, by emissions of plane or circular wavefronts, allows severalfold increase in frame rates. Conventional and ultrafast color Doppler are both limited by the range-velocity dilemma, which may result in velocity folding (aliasing) for large depths and/or large velocities. We investigated multiple pulse-repetition-frequency (PRF) emissions arranged in a series of staggered intervals to remove aliasing in ultrafast color Doppler. Staggered PRF is an emission process where time delays between successive pulse transmissions change in an alternating way. We tested staggered dual- and triple-PRF ultrafast color Doppler, 1) in vitro in a spinning disc and a free jet flow, and 2) in vivo in a human left ventricle. The in vitro results showed that the Nyquist velocity could be extended to up to 6 times the conventional limit. We found coefficients of determination r(2) ≥ 0.98 between the de-aliased and ground-truth velocities. Consistent de-aliased Doppler images were also obtained in the human left heart. Our results demonstrate that staggered multiple-PRF ultrafast color Doppler is efficient for high-velocity high-frame-rate blood flow imaging. This is particularly relevant for new developments in ultrasound imaging relying on accurate velocity measurements.

Theoretical study of sum-frequency vibrational spectroscopy on limonene surface

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

Zheng, Ren-Hui, E-mail: zrh@iccas.ac.cn; Liu, Hao; Jing, Yuan-Yuan

2014-03-14

By combining molecule dynamics (MD) simulation and quantum chemistry computation, we calculate the surface sum-frequency vibrational spectroscopy (SFVS) of R-limonene molecules at the gas-liquid interface for SSP, PPP, and SPS polarization combinations. The distributions of the Euler angles are obtained using MD simulation, the ψ-distribution is between isotropic and Gaussian. Instead of the MD distributions, different analytical distributions such as the δ-function, Gaussian and isotropic distributions are applied to simulate surface SFVS. We find that different distributions significantly affect the absolute SFVS intensity and also influence on relative SFVS intensity, and the δ-function distribution should be used with caution whenmore » the orientation distribution is broad. Furthermore, the reason that the SPS signal is weak in reflected arrangement is discussed.« less

Surface Displacement Measurements, Strain and Vibrational Analysis using Speckle Metrology Techniques.

DTIC Science & Technology

1980-03-01

Ennos, A. E., " Measurement by Laser Photography," National Physical Laboratory, Division of Optical Metrology, Teddington, Middlesex, U.K. 9. Archbold...Field Measurement ," Optics and Laser TechnoloZ, pp. 216 - 219, October 1776. 149 37. Khetan, R. P., and Chiang, F. P., "Strain Analysis by One Beam...AD-AO85 145 NAVAL POSTGRADUATE SCHOOL MONTEREY CA F/G 17/8 SURFACE DISPLACEMENT MEASUREMENTS , STRAIN AND VIBRATIONAL ANALY-ETC(U) MAR GO A B

Vibration dampener for dampening vibration of a tubular member

DOEpatents

Obermeyer, F.D.; Middlebrooks, W.B.; DeMario, E.E.

1994-10-18

Vibration dampener for dampening vibration of a tubular member, such as an instrumentation tube of the type found in nuclear reactor pressure vessels is disclosed. The instrumentation tube is received in an outer tubular member, such as a guide thimble tube. The vibration dampener comprises an annular sleeve which is attachable to the inside surface of the guide thimble tube and which is sized to surround the instrumentation tube. Dimples are attached to the interior wall of the sleeve for radially supporting the instrumentation tube. The wall of the sleeve has a flexible spring member, which is formed from the wall, disposed opposite the dimples for biasing the instrumentation tube into abutment with the dimples. Flow-induced vibration of the instrumentation tube will cause it to move out of contact with the dimples and further engage the spring member, which will flex a predetermined amount and exert a reactive force against the instrumentation tube to restrain its movement. The amount by which the spring member will flex is less than the unrestrained amplitude of vibration of the instrumentation tube. The reactive force exerted against the instrumentation tube will be sufficient to return it to its original axial position within the thimble tube. In this manner, vibration of the instrumentation tube is dampened so that in-core physics measurements are accurate and so that the instrumentation tube will not wear against the inside surface of the guide thimble tube. 14 figs.

Vibration dampener for dampening vibration of a tubular member

DOEpatents

Obermeyer, Franklin D.; Middlebrooks, Willis B.; DeMario, Edmund E.

1994-01-01

Vibration dampener for dampening vibration of a tubular member, such as an instrumentation tube of the type found in nuclear reactor pressure vessels. The instrumentation tube is received in an outer tubular member, such as a guide thimble tube. The vibration dampener comprises an annular sleeve which is attachable to the inside surface of the guide thimble tube and which is sized to surround the instrumentation tube. Dimples are attached to the interior wall of the sleeve for radially supporting the instrumentation tube. The wall of the sleeve has a flexible spring member, which is formed from the wall, disposed opposite the dimples for biasing the instrumentation tube into abutment with the dimples. Flow-induced vibration of the instrumentation tube will cause it to move out of contact with the dimples and further engage the spring member, which will flex a predetermined amount and exert a reactive force against the instrumentation tube to restrain its movement. The amount by which the spring member will flex is less than the unrestrained amplitude of vibration of the instrumentation tube. The reactive force exerted against the instrumentation tube will be sufficient to return it to its original axial position within the thimble tube. In this manner, vibration of the instrumentation tube is dampened so that in-core physics measurements are accurate and so that the instrumentation tube will not wear against the inside surface of the guide thimble tube.

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

4-D ultrafast shear-wave imaging.

PubMed

Gennisson, Jean-Luc; Provost, Jean; Deffieux, Thomas; Papadacci, Clément; Imbault, Marion; Pernot, Mathieu; Tanter, Mickael

2015-06-01

Over the last ten years, shear wave elastography (SWE) has seen considerable development and is now routinely used in clinics to provide mechanical characterization of tissues to improve diagnosis. The most advanced technique relies on the use of an ultrafast scanner to generate and image shear waves in real time in a 2-D plane at several thousands of frames per second. We have recently introduced 3-D ultrafast ultrasound imaging to acquire with matrix probes the 3-D propagation of shear waves generated by a dedicated radiation pressure transducer in a single acquisition. In this study, we demonstrate 3-D SWE based on ultrafast volumetric imaging in a clinically applicable configuration. A 32 × 32 matrix phased array driven by a customized, programmable, 1024-channel ultrasound system was designed to perform 4-D shear-wave imaging. A matrix phased array was used to generate and control in 3-D the shear waves inside the medium using the acoustic radiation force. The same matrix array was used with 3-D coherent plane wave compounding to perform high-quality ultrafast imaging of the shear wave propagation. Volumetric ultrafast acquisitions were then beamformed in 3-D using a delay-and-sum algorithm. 3-D volumetric maps of the shear modulus were reconstructed using a time-of-flight algorithm based on local multiscale cross-correlation of shear wave profiles in the three main directions using directional filters. Results are first presented in an isotropic homogeneous and elastic breast phantom. Then, a full 3-D stiffness reconstruction of the breast was performed in vivo on healthy volunteers. This new full 3-D ultrafast ultrasound system paves the way toward real-time 3-D SWE.

Generalized GW+Boltzmann Approach for the Description of Ultrafast Electron Dynamics in Topological Insulators

PubMed Central

Battiato, Marco; Sánchez-Barriga, Jaime

2017-01-01

Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin–orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized GW+Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron–electron and electron–phonon scatterings. Taking the prototypical insulator Bi2Te3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron–electron and electron–phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials. PMID:28773171

Generalized GW+Boltzmann Approach for the Description of Ultrafast Electron Dynamics in Topological Insulators.

PubMed

Battiato, Marco; Aguilera, Irene; Sánchez-Barriga, Jaime

2017-07-17

Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin-orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized G W +Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron-electron and electron-phonon scatterings. Taking the prototypical insulator Bi 2 Te 3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron-electron and electron-phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials.

Theory of H bonding and vibration on close-packed metal surfaces

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

Feibelman, P.J.; Hamann, D.R.

1987-07-01

Self-consistent linearized augmented plane-wave calculations for H monolayers adsorbed on Pt(111), Ru(0001), Cu(111), and Cu(1 x 1)/Ru(0001) thin slabs predict the following: the H-atom equilibrium position on these substrates is generally in the face-centered cubic threefold hollow at a height above the surface where the clean-metal electron density is about 0.015 a.u. The symmetric stretch (SS) frequency lies in the range 130--165 meV, and is about 30% greater than the asymmetric stretch (AS) frequency on the same substrate. These results contradict the mode assignments of Baro et al. (A. M. Baro, H. Ibach, and H. D. Bruchman, Surf. Sci. 88,more » 384 (1979)) for H/Pt(111) which were based on the observation of weak dipole scattering by the low-lying mode, and of Barteau et al. (M. A. Barteau, J. Q. Broughton, and D. Menzel, Surf. Sci. 133, 443 (1983)) for H/Ru(0001). The pairwise spring model of H--metal vibration invoked by these groups in support of their mode assignments neglects a major component of the H--metal interaction, that between the adsorbed H and the delocalized electrons of a metal surface. It is this interaction which is responsible for the fact that the frequency of the SS vibration is greater than that of the AS.« less

Three-Dimensional Solution of the Free Vibration Problem for Metal-Ceramic Shells Using the Method of Sampling Surfaces

NASA Astrophysics Data System (ADS)

Kulikov, G. M.; Plotnikova, S. V.

2017-03-01

The possibility of using the method of sampling surfaces (SaS) for solving the free vibration problem of threedimensional elasticity for metal-ceramic shells is studied. According to this method, in the shell body, an arbitrary number of SaS parallel to its middle surface are selected in order to take displacements of these surfaces as unknowns. The SaS pass through the nodes of a Chebyshev polynomial, which improves the convergence of the SaS method significantly. As a result, the SaS method can be used to obtain analytical solutions of the vibration problem for metal-ceramic plates and cylindrical shells that asymptotically approach the exact solutions of elasticity as the number of SaS tends to infinity.

Mechanical vibration of viscoelastic liquid droplets

NASA Astrophysics Data System (ADS)

Sharp, James; Harrold, Victoria

2014-03-01

The resonant vibrations of viscoelastic sessile droplets supported on different substrates were monitored using a simple laser light scattering technique. In these experiments, laser light was reflected from the surfaces of droplets of high Mw poly acrylamide-co-acrylic acid (PAA) dissolved in water. The scattered light was allowed to fall on the surface of a photodiode detector and a mechanical impulse was applied to the drops using a vibration motor mounted beneath the substrates. The mechanical impulse caused the droplets to vibrate and the scattered light moved across the surface of the photodiode. The resulting time dependent photodiode signal was then Fourier transformed to obtain the mechanical vibrational spectra of the droplets. The frequencies and widths of the resonant peaks were extracted for droplets containing different concentrations of PAA and with a range of sizes. This was repeated for PAA loaded water drops on surfaces which displayed different values of the three phase contact angle. The results were compared to a simple model of droplet vibration which considers the formation of standing wave states on the surface of a viscoelastic droplet. We gratefully acknowledge the support of the Leverhulme trust under grant number RPG-2012-702.

Surface vibrational relaxation of N2 studied by infrared titration with time resolved Quantum Cascade Laser diagnostics

NASA Astrophysics Data System (ADS)

Marinov, D.; Guaitella, O.; Rousseau, A.; Lopatik, D.; Hübner, M.; Röpcke, J.; Ionikh, Yu

2012-10-01

Relaxation of vibrationally excited nitrogen molecules on reactor walls is the most efficient N2(v) loss mechanism in laboratory plasmas at pressures up to few tens of mbars. In the present study a new method for determination of the de-excitation probability γN2 of vibrationally excited N2 on different surfaces has been developed. A short dc discharge pulse was applied to a mixture containing 0.05-1% of CO2, N2O or CO in N2 at 1.3 mbar. Due to a very efficient vibrational coupling between N2(v) and CO2 (N2O, CO), the vibrational excitation of these titrating molecules is an image of the vibrational excitation of N2. In the afterglow, the vibrational relaxation was monitored in-situ using quantum cascade laser absorption spectroscopy. The measurements were performed in a single discharge pulse without signal accumulation. Experimental results were interpreted in terms of a numerical model of non-equilibrium vibrational kinetics. The value of γN2 was determined from the best agreement between the measured and calculated relaxation times. Using new technique the relaxation probability of N2(v) was measured for SiO2, TiO2, Al2O3, Pyrex and anodized aluminum.

Simulation of X-ray transient absorption for following vibrations in coherently ionized F2 molecules

NASA Astrophysics Data System (ADS)

Dutoi, Anthony D.; Leone, Stephen R.

2017-01-01

Femtosecond and attosecond X-ray transient absorption experiments are becoming increasingly sophisticated tools for probing nuclear dynamics. In this work, we explore and develop theoretical tools needed for interpretation of such spectra,in order to characterize the vibrational coherences that result from ionizing a molecule in a strong IR field. Ab initio data for F2 is combined with simulations of nuclear dynamics, in order to simulate time-resolved X-ray absorption spectra for vibrational wavepackets after coherent ionization at 0 K and at finite temperature. Dihalogens pose rather difficult electronic structure problems, and the issues encountered in this work will be reflective of those encountered with any core-valence excitation simulation when a bond is breaking. The simulations reveal a strong dependence of the X-ray absorption maximum on the locations of the vibrational wave packets. A Fourier transform of the simulated signal shows features at the overtone frequencies of both the neutral and the cation, which reflect spatial interferences of the vibrational eigenstates. This provides a direct path for implementing ultrafast X-ray spectroscopic methods to visualize coherent nuclear dynamics.

Adsorption and desorption of hydrogen at nonpolar GaN (1 1 ¯ 00 ) surfaces: Kinetics and impact on surface vibrational and electronic properties

NASA Astrophysics Data System (ADS)

Lymperakis, L.; Neugebauer, J.; Himmerlich, M.; Krischok, S.; Rink, M.; Kröger, J.; Polyakov, V. M.

2017-05-01

The adsorption of hydrogen at nonpolar GaN (1 1 ¯00 ) surfaces and its impact on the electronic and vibrational properties is investigated using surface electron spectroscopy in combination with density functional theory (DFT) calculations. For the surface mediated dissociation of H2 and the subsequent adsorption of H, an energy barrier of 0.55 eV has to be overcome. The calculated kinetic surface phase diagram indicates that the reaction is kinetically hindered at low pressures and low temperatures. At higher temperatures ab initio thermodynamics show, that the H-free surface is energetically favored. To validate these theoretical predictions experiments at room temperature and under ultrahigh vacuum conditions were performed. They reveal that molecular hydrogen does not dissociatively adsorb at the GaN (1 1 ¯00 ) surface. Only activated atomic hydrogen atoms attach to the surface. At temperatures above 820 K, the attached hydrogen gets desorbed. The adsorbed hydrogen atoms saturate the dangling bonds of the gallium and nitrogen surface atoms and result in an inversion of the Ga-N surface dimer buckling. The signatures of the Ga-H and N-H vibrational modes on the H-covered surface have experimentally been identified and are in good agreement with the DFT calculations of the surface phonon modes. Both theory and experiment show that H adsorption results in a removal of occupied and unoccupied intragap electron states of the clean GaN (1 1 ¯00 ) surface and a reduction of the surface upward band bending by 0.4 eV. The latter mechanism largely reduces surface electron depletion.

Ultrafast fiber lasers: practical applications

NASA Astrophysics Data System (ADS)

Pastirk, Igor; Sell, Alexander; Herda, Robert; Brodschelm, Andreas; Zach, Armin

2015-05-01

Over past three decades ultrafast lasers have come a long way from the bulky, demanding and very sensitive scientific research projects to widely available commercial products. For the majority of this period the titanium-sapphire-based ultrafast systems were the workhorse for scientific and emerging industrial and biomedical applications. However the complexity and intrinsic bulkiness of solid state lasers have prevented even larger penetration into wider array of practical applications. With emergence of femtosecond fiber lasers, based primarily on Er-doped and Yb-doped fibers that provide compact, inexpensive and dependable fs and ps pulses, new practical applications have become a reality. The overview of current state of the art ultrafast fiber sources, their basic principles and most prominent applications will be presented, including micromachining and biomedical implementations (ophthalmology) on one end of the pulse energy spectrum and 3D lithography and THz applications on the other.

Ultrafast infrared spectroscopy reveals water-mediated coherent dynamics in an enzyme active site.

PubMed

Adamczyk, Katrin; Simpson, Niall; Greetham, Gregory M; Gumiero, Andrea; Walsh, Martin A; Towrie, Michael; Parker, Anthony W; Hunt, Neil T

2015-01-01

Understanding the impact of fast dynamics upon the chemical processes occurring within the active sites of proteins and enzymes is a key challenge that continues to attract significant interest, though direct experimental insight in the solution phase remains sparse. Similar gaps in our knowledge exist in understanding the role played by water, either as a solvent or as a structural/dynamic component of the active site. In order to investigate further the potential biological roles of water, we have employed ultrafast multidimensional infrared spectroscopy experiments that directly probe the structural and vibrational dynamics of NO bound to the ferric haem of the catalase enzyme from Corynebacterium glutamicum in both H 2 O and D 2 O. Despite catalases having what is believed to be a solvent-inaccessible active site, an isotopic dependence of the spectral diffusion and vibrational lifetime parameters of the NO stretching vibration are observed, indicating that water molecules interact directly with the haem ligand. Furthermore, IR pump-probe data feature oscillations originating from the preparation of a coherent superposition of low-frequency vibrational modes in the active site of catalase that are coupled to the haem ligand stretching vibration. Comparisons with an exemplar of the closely-related peroxidase enzyme family shows that they too exhibit solvent-dependent active-site dynamics, supporting the presence of interactions between the haem ligand and water molecules in the active sites of both catalases and peroxidases that may be linked to proton transfer events leading to the formation of the ferryl intermediate Compound I. In addition, a strong, water-mediated, hydrogen bonding structure is suggested to occur in catalase that is not replicated in peroxidase; an observation that may shed light on the origins of the different functions of the two enzymes.

Vibrational Mode-Specific Reaction of Methane on a Nickel Surface

NASA Astrophysics Data System (ADS)

Beck, Rainer D.; Maroni, Plinio; Papageorgopoulos, Dimitrios C.; Dang, Tung T.; Schmid, Mathieu P.; Rizzo, Thomas R.

2003-10-01

The dissociation of methane on a nickel catalyst is a key step in steam reforming of natural gas for hydrogen production. Despite substantial effort in both experiment and theory, there is still no atomic-scale description of this important gas-surface reaction. We report quantum state-resolved studies, using pulsed laser and molecular beam techniques, of vibrationally excited methane reacting on the nickel (100) surface. For doubly deuterated methane (CD2H2), we observed that the reaction probability with two quanta of excitation in one C-H bond was greater (by as much as a factor of 5) than with one quantum in each of two C-H bonds. These results clearly exclude the possibility of statistical models correctly describing the mechanism of this process and attest to the importance of full-dimensional calculations of the reaction dynamics.

Vibrational mode-specific reaction of methane on a nickel surface.

PubMed

Beck, Rainer D; Maroni, Plinio; Papageorgopoulos, Dimitrios C; Dang, Tung T; Schmid, Mathieu P; Rizzo, Thomas R

2003-10-03

The dissociation of methane on a nickel catalyst is a key step in steam reforming of natural gas for hydrogen production. Despite substantial effort in both experiment and theory, there is still no atomic-scale description of this important gas-surface reaction. We report quantum state-resolved studies, using pulsed laser and molecular beam techniques, of vibrationally excited methane reacting on the nickel (100) surface. For doubly deuterated methane (CD2H2), we observed that the reaction probability with two quanta of excitation in one C-H bond was greater (by as much as a factor of 5) than with one quantum in each of two C-H bonds. These results clearly exclude the possibility of statistical models correctly describing the mechanism of this process and attest to the importance of full-dimensional calculations of the reaction dynamics.

Vibrational energies for HFCO using a neural network sum of exponentials potential energy surface

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

Pradhan, Ekadashi; Brown, Alex, E-mail: alex.brown@ualberta.ca

2016-05-07

A six-dimensional potential energy surface (PES) for formyl fluoride (HFCO) is fit in a sum-of-products form using neural network exponential fitting functions. The ab initio data upon which the fit is based were computed at the explicitly correlated coupled cluster with single, double, and perturbative triple excitations [CCSD(T)-F12]/cc-pVTZ-F12 level of theory. The PES fit is accurate (RMSE = 10 cm{sup −1}) up to 10 000 cm{sup −1} above the zero point energy and covers most of the experimentally measured IR data. The PES is validated by computing vibrational energies for both HFCO and deuterated formyl fluoride (DFCO) using block improved relaxationmore » with the multi-configuration time dependent Hartree approach. The frequencies of the fundamental modes, and all other vibrational states up to 5000 cm{sup −1} above the zero-point energy, are more accurate than those obtained from the previous MP2-based PES. The vibrational frequencies obtained on the PES are compared to anharmonic frequencies at the MP2/aug-cc-pVTZ and CCSD(T)/aug-cc-pVTZ levels of theory obtained using second-order vibrational perturbation theory. The new PES will be useful for quantum dynamics simulations for both HFCO and DFCO, e.g., studies of intramolecular vibrational redistribution leading to unimolecular dissociation and its laser control.« less

Effect of Vibration Training on Anaerobic Power and Quardroceps Surface EMG in Long Jumpers

ERIC Educational Resources Information Center

Liu, Bin; Luo, Jiong

2015-01-01

Objective: To explore the anaerobic power and surface EMG (sEMG) of quardrocep muscle in lower extremities after single vibration training intervention. Methods: 8 excellent male long jumpers voluntarily participated in this study. Four intervention modes were devised, including high frequency high amplitude (HFHA,30Hz,6mm), low frequency low…

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.

Relaxation dynamics and coherent energy exchange in coupled vibration-cavity polaritons (Conference Presentation)

NASA Astrophysics Data System (ADS)

Simpkins, Blake S.; Fears, Kenan P.; Dressick, Walter J.; Dunkelberger, Adam D.; Spann, Bryan T.; Owrutsky, Jeffrey C.

2016-09-01

Coherent coupling between an optical transition and confined optical mode have been investigated for electronic-state transitions, however, only very recently have vibrational transitions been considered. Here, we demonstrate both static and dynamic results for vibrational bands strongly coupled to optical cavities. We experimentally and numerically describe strong coupling between a Fabry-Pérot cavity and carbonyl stretch ( 1730 cm 1) in poly-methylmethacrylate and provide evidence that the mixed-states are immune to inhomogeneous broadening. We investigate strong and weak coupling regimes through examination of cavities loaded with varying concentrations of a urethane monomer. Rabi splittings are in excellent agreement with an analytical description using no fitting parameters. Ultrafast pump-probe measurements reveal transient absorption signals over a frequency range well-separated from the vibrational band, as well as drastically modified relaxation rates. We speculate these modified kinetics are a consequence of the energy proximity between the vibration-cavity polariton modes and excited state transitions and that polaritons offer an alternative relaxation path for vibrational excitations. Varying the polariton energies by angle-tuning yields transient results consistent with this hypothesis. Furthermore, Rabi oscillations, or quantum beats, are observed at early times and we see evidence that these coherent vibration-cavity polariton excitations impact excited state population through cavity losses. Together, these results indicate that cavity coupling may be used to influence both excitation and relaxation rates of vibrations. Opening the field of polaritonic coupling to vibrational species promises to be a rich arena amenable to a wide variety of infrared-active bonds that can be studied in steady state and dynamically.

Roadmap of ultrafast x-ray atomic and molecular physics

NASA Astrophysics Data System (ADS)

Young, Linda; Ueda, Kiyoshi; Gühr, Markus; Bucksbaum, Philip H.; Simon, Marc; Mukamel, Shaul; Rohringer, Nina; Prince, Kevin C.; Masciovecchio, Claudio; Meyer, Michael; Rudenko, Artem; Rolles, Daniel; Bostedt, Christoph; Fuchs, Matthias; Reis, David A.; Santra, Robin; Kapteyn, Henry; Murnane, Margaret; Ibrahim, Heide; Légaré, François; Vrakking, Marc; Isinger, Marcus; Kroon, David; Gisselbrecht, Mathieu; L'Huillier, Anne; Wörner, Hans Jakob; Leone, Stephen R.

2018-02-01

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm-2) of x-rays at wavelengths down to ˜1 Ångstrom, and HHG provides unprecedented time resolution (˜50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ˜280 eV (44 Ångstroms) and the bond length in methane of ˜1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since

Roadmap of ultrafast x-ray atomic and molecular physics

DOE PAGES

Young, Linda; Ueda, Kiyoshi; Gühr, Markus; ...

2018-01-09

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (10 20 W cm -2) of x-rays at wavelengths down to ~1 Ångstrom, and HHG provides unprecedented time resolution (~50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scalesmore » can be referenced to the chemically significant carbon K-edge at a photon energy of ~280 eV (44 Ångstroms) and the bond length in methane of ~1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities

Roadmap of ultrafast x-ray atomic and molecular physics

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

Young, Linda; Ueda, Kiyoshi; Gühr, Markus

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (10 20 W cm -2) of x-rays at wavelengths down to ~1 Ångstrom, and HHG provides unprecedented time resolution (~50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scalesmore » can be referenced to the chemically significant carbon K-edge at a photon energy of ~280 eV (44 Ångstroms) and the bond length in methane of ~1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities

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.

Material processing with fiber based ultrafast pulse delivery

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

Effect of flask vibration time on casting integrity, Surface Penetration and Coating Inclusion in lost foam casting of Al-Si Alloy

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

Karimian, Majid; Idris, M. H.; Ourdjini, A.

2011-01-17

The paper presents the result of an experimental investigation conducted on medium aluminum silicon alloy casting- LM6, using no-vacuum assisted lost foam casting process. The study is directed for establishing the relationship between the flask vibrations times developed for molded sample on the casting integrity, surface penetration and coating inclusion defects of the casting. Four different flask vibration times namely 180, 120, 90 and 60 sec. were investigated. The casting integrity was investigated in terms of fulfilling in all portions and edges. The surface penetration was measured using optical microscope whilst image analyzer was used to quantify the percentage ofmore » coating inclusion in the casting. The results show that vibration time has significant influence on the fulfilling as well as the internal integrity of the lost foam casting. It was found that the lower vibration time produced comparatively sound casing.« less

Full skin quantitative optical coherence elastography achieved by combining vibration and surface acoustic wave methods

NASA Astrophysics Data System (ADS)

Li, Chunhui; Guan, Guangying; Huang, Zhihong; Wang, Ruikang K.; Nabi, Ghulam

2015-03-01

By combining with the phase sensitive optical coherence tomography (PhS-OCT), vibration and surface acoustic wave (SAW) methods have been reported to provide elastography of skin tissue respectively. However, neither of these two methods can provide the elastography in full skin depth in current systems. This paper presents a feasibility study on an optical coherence elastography method which combines both vibration and SAW in order to give the quantitative mechanical properties of skin tissue with full depth range, including epidermis, dermis and subcutaneous fat. Experiments are carried out on layered tissue mimicking phantoms and in vivo human forearm and palm skin. A ring actuator generates vibration while a line actuator were used to excited SAWs. A PhS-OCT system is employed to provide the ultrahigh sensitive measurement of the generated waves. The experimental results demonstrate that by the combination of vibration and SAW method the full skin bulk mechanical properties can be quantitatively measured and further the elastography can be obtained with a sensing depth from ~0mm to ~4mm. This method is promising to apply in clinics where the quantitative elasticity of localized skin diseases is needed to aid the diagnosis and treatment.

Vibrational fingerprinting of bacterial pathogens by surface enhanced Raman scattering (SERS)

NASA Astrophysics Data System (ADS)

Premasiri, W. Ranjith; Moir, D. T.; Ziegler, Lawrence D.

2005-05-01

The surface enhanced Raman scattering (SERS) spectra of vegetative whole-cell bacteria were obtained using in-situ grown gold nanoparticle cluster-covered silicon dioxide substrates excited at 785 nm. SERS spectra of Gram-negative bacteria; E. coli and S. typhimurium, and Gram-positive bacteria; B. subtilis, B. cereus, B. thuringeinsis and B. anthracis Sterne, have been observed. Raman enhancement factors of ~104-105 per cell are found for both Gram positive and Gram negative bacteria on this novel SERS substrate. The bacterial SERS spectra are species specific and exhibit greater species differentiation and reduced spectral congestion than their corresponding non-SERS (bulk) Raman spectra. Fluorescence observed in the 785 nm excited bulk Raman emission of Bacillus species is not apparent in the corresponding SERS spectra. The surface enhancement effect allows the observation of Raman spectra at the single cell level excited by low incident laser powers (< 3 mW) and short data acquisition times (~20 sec.). Comparison with previous SERS studies suggests that these SERS vibrational signatures are sensitively dependent on the specific morphology and nature of the SERS active substrate. Exposure to biological environments, such as human blood serum, has an observable effect on the bacterial SERS spectra. However, reproducible, species specific SERS vibrational fingerprints are still obtained. The potential of SERS for detection and identification of bacteria with species specificity on these gold nanoparticle coated substrates is demonstrated by these results.

Vibration mode imaging.

PubMed

Zhang, Xiaoming; Zeraati, Mohammad; Kinnick, Randall R; Greenleaf, James F; Fatemi, Mostafa

2007-06-01

A new method for imaging the vibration mode of an object is investigated. The radiation force of ultrasound is used to scan the object at a resonant frequency of the object. The vibration of the object is measured by laser and the resulting acoustic emission from the object is measured by a hydrophone. It is shown that the measured signal is proportional to the value of the mode shape at the focal point of the ultrasound beam. Experimental studies are carried out on a mechanical heart valve and arterial phantoms. The mode images on the valve are made by the hydrophone measurement and confirmed by finite-element method simulations. Compared with conventional B-scan imaging on arterial phantoms, the mode imaging can show not only the interface of the artery and the gelatin, but also the vibration modes of the artery. The images taken on the phantom surface suggest that an image of an interior artery can be made by vibration measurements on the surface of the body. However, the image of the artery can be improved if the vibration of the artery is measured directly. Imaging of the structure in the gelatin or tissue can be enhanced by small bubbles and contrast agents.

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.

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

Hydration and vibrational dynamics of betaine (N,N,N-trimethylglycine)

NASA Astrophysics Data System (ADS)

Li, Tanping; Cui, Yaowen; Mathaga, John; Kumar, Revati; Kuroda, Daniel G.

2015-06-01

Zwitterions are naturally occurring molecules that have a positive and a negative charge group in its structure and are of great importance in many areas of science. Here, the vibrational and hydration dynamics of the zwitterionic system betaine (N,N,N-trimethylglycine) is reported. The linear infrared spectrum of aqueous betaine exhibits an asymmetric band in the 1550-1700 cm-1 region of the spectrum. This band is attributed to the carboxylate asymmetric stretch of betaine. The potential of mean force computed from ab initio molecular dynamic simulations confirms that the two observed transitions of the linear spectrum are related to two different betaine conformers present in solution. A model of the experimental data using non-linear response theory agrees very well with a vibrational model comprising of two vibrational transitions. In addition, our modeling shows that spectral parameters such as the slope of the zeroth contour plot and central line slope are both sensitive to the presence of overlapping transitions. The vibrational dynamics of the system reveals an ultrafast decay of the vibrational population relaxation as well as the correlation of frequency-frequency correlation function (FFCF). A decay of ˜0.5 ps is observed for the FFCF correlation time and is attributed to the frequency fluctuations caused by the motions of water molecules in the solvation shell. The comparison of the experimental observations with simulations of the FFCF from ab initio molecular dynamics and a density functional theory frequency map shows a very good agreement corroborating the correct characterization and assignment of the derived parameters.

Hydration and vibrational dynamics of betaine (N,N,N-trimethylglycine)

PubMed Central

Li, Tanping; Cui, Yaowen; Mathaga, John; Kumar, Revati; Kuroda, Daniel G.

2015-01-01

Zwitterions are naturally occurring molecules that have a positive and a negative charge group in its structure and are of great importance in many areas of science. Here, the vibrational and hydration dynamics of the zwitterionic system betaine (N,N,N-trimethylglycine) is reported. The linear infrared spectrum of aqueous betaine exhibits an asymmetric band in the 1550-1700 cm−1 region of the spectrum. This band is attributed to the carboxylate asymmetric stretch of betaine. The potential of mean force computed from ab initio molecular dynamic simulations confirms that the two observed transitions of the linear spectrum are related to two different betaine conformers present in solution. A model of the experimental data using non-linear response theory agrees very well with a vibrational model comprising of two vibrational transitions. In addition, our modeling shows that spectral parameters such as the slope of the zeroth contour plot and central line slope are both sensitive to the presence of overlapping transitions. The vibrational dynamics of the system reveals an ultrafast decay of the vibrational population relaxation as well as the correlation of frequency-frequency correlation function (FFCF). A decay of ∼0.5 ps is observed for the FFCF correlation time and is attributed to the frequency fluctuations caused by the motions of water molecules in the solvation shell. The comparison of the experimental observations with simulations of the FFCF from ab initio molecular dynamics and a density functional theory frequency map shows a very good agreement corroborating the correct characterization and assignment of the derived parameters. PMID:26049458

Mechanism of vibrational energy dissipation of free OH groups at the air-water interface.

PubMed

Hsieh, Cho-Shuen; Campen, R Kramer; Okuno, Masanari; Backus, Ellen H G; Nagata, Yuki; Bonn, Mischa

2013-11-19

Interfaces of liquid water play a critical role in a wide variety of processes that occur in biology, a variety of technologies, and the environment. Many macroscopic observations clarify that the properties of liquid water interfaces significantly differ from those of the bulk liquid. In addition to interfacial molecular structure, knowledge of the rates and mechanisms of the relaxation of excess vibrational energy is indispensable to fully understand physical and chemical processes of water and aqueous solutions, such as chemical reaction rates and pathways, proton transfer, and hydrogen bond dynamics. Here we elucidate the rate and mechanism of vibrational energy dissipation of water molecules at the air-water interface using femtosecond two-color IR-pump/vibrational sum-frequency probe spectroscopy. Vibrational relaxation of nonhydrogen-bonded OH groups occurs at a subpicosecond timescale in a manner fundamentally different from hydrogen-bonded OH groups in bulk, through two competing mechanisms: intramolecular energy transfer and ultrafast reorientational motion that leads to free OH groups becoming hydrogen bonded. Both pathways effectively lead to the transfer of the excited vibrational modes from free to hydrogen-bonded OH groups, from which relaxation readily occurs. Of the overall relaxation rate of interfacial free OH groups at the air-H2O interface, two-thirds are accounted for by intramolecular energy transfer, whereas the remaining one-third is dominated by the reorientational motion. These findings not only shed light on vibrational energy dynamics of interfacial water, but also contribute to our understanding of the impact of structural and vibrational dynamics on the vibrational sum-frequency line shapes of aqueous interfaces.

Ultrafast strong broadband light source generated in nanoscale plasmonic Au-AAO-Al structures

NASA Astrophysics Data System (ADS)

Han, Junbo; Yao, Linhua; Ma, Zongwei

we demonstrate an ultrafast strong broadband photoluminescence (PL) from Au-AAO-Al composite under low excitation power intensity of 3.8 34.5 GW /cm2. The emission wavelength is in the range of 450-1050 nm and the lifetime is under sub-nanosecond. Comparative studies of PL in Au-AAO-Al with different Au rod length and Au-AAO without Al coupling layer, together with the finite difference time domain (FDTD) calculations, present that the fast PL originates from the surface plasmon enhanced supercontinuum generation (SCG) in AAO membrane. The observations indicate that strong SCG could be realized in nanoscale plasmonic structures, which have promise applications in the minimization and integration of ultrafast lighting sources in photonic devices. National Natural Scientific Foundation of China (11404124).

3D ultrafast ultrasound imaging in vivo.

PubMed

Provost, Jean; Papadacci, Clement; Arango, Juan Esteban; Imbault, Marion; Fink, Mathias; Gennisson, Jean-Luc; Tanter, Mickael; Pernot, Mathieu

2014-10-07

Very high frame rate ultrasound imaging has recently allowed for the extension of the applications of echography to new fields of study such as the functional imaging of the brain, cardiac electrophysiology, and the quantitative imaging of the intrinsic mechanical properties of tumors, to name a few, non-invasively and in real time. In this study, we present the first implementation of Ultrafast Ultrasound Imaging in 3D based on the use of either diverging or plane waves emanating from a sparse virtual array located behind the probe. It achieves high contrast and resolution while maintaining imaging rates of thousands of volumes per second. A customized portable ultrasound system was developed to sample 1024 independent channels and to drive a 32  ×  32 matrix-array probe. Its ability to track in 3D transient phenomena occurring in the millisecond range within a single ultrafast acquisition was demonstrated for 3D Shear-Wave Imaging, 3D Ultrafast Doppler Imaging, and, finally, 3D Ultrafast combined Tissue and Flow Doppler Imaging. The propagation of shear waves was tracked in a phantom and used to characterize its stiffness. 3D Ultrafast Doppler was used to obtain 3D maps of Pulsed Doppler, Color Doppler, and Power Doppler quantities in a single acquisition and revealed, at thousands of volumes per second, the complex 3D flow patterns occurring in the ventricles of the human heart during an entire cardiac cycle, as well as the 3D in vivo interaction of blood flow and wall motion during the pulse wave in the carotid at the bifurcation. This study demonstrates the potential of 3D Ultrafast Ultrasound Imaging for the 3D mapping of stiffness, tissue motion, and flow in humans in vivo and promises new clinical applications of ultrasound with reduced intra--and inter-observer variability.

Vibrations that live long and prosper

NASA Astrophysics Data System (ADS)

Utz, Arthur L.

2018-06-01

Molecular vibrations can be highly effective promoters of gas-phase chemistry. Now, measurements show that excited vibrational states can survive on metal surfaces far longer than expected — reshaping our understanding of how vibrational excitation might also promote or modify heterogeneously catalysed chemistry on metals.

Perspective: Ultrafast magnetism and THz spintronics

NASA Astrophysics Data System (ADS)

Walowski, Jakob; Münzenberg, Markus

2016-10-01

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

Perspective: Ultrafast magnetism and THz spintronics

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

Walowski, Jakob; Münzenberg, Markus

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

High fidelity quantum gates with vibrational qubits.

PubMed

Berrios, Eduardo; Gruebele, Martin; Shyshlov, Dmytro; Wang, Lei; Babikov, Dmitri

2012-11-26

Physical implementation of quantum gates acting on qubits does not achieve a perfect fidelity of 1. The actual output qubit may not match the targeted output of the desired gate. According to theoretical estimates, intrinsic gate fidelities >99.99% are necessary so that error correction codes can be used to achieve perfect fidelity. Here we test what fidelity can be accomplished for a CNOT gate executed by a shaped ultrafast laser pulse interacting with vibrational states of the molecule SCCl(2). This molecule has been used as a test system for low-fidelity calculations before. To make our test more stringent, we include vibrational levels that do not encode the desired qubits but are close enough in energy to interfere with population transfer by the laser pulse. We use two complementary approaches: optimal control theory determines what the best possible pulse can do; a more constrained physical model calculates what an experiment likely can do. Optimal control theory finds pulses with fidelity >0.9999, in excess of the quantum error correction threshold with 8 × 10(4) iterations. On the other hand, the physical model achieves only 0.9992 after 8 × 10(4) iterations. Both calculations converge as an inverse power law toward unit fidelity after >10(2) iterations/generations. In principle, the fidelities necessary for quantum error correction are reachable with qubits encoded by molecular vibrations. In practice, it will be challenging with current laboratory instrumentation because of slow convergence past fidelities of 0.99.

Effects of Achilles tendon vibration, surface and visual conditions on lower leg electromyography in young adults with and without recurrent ankle sprains.

PubMed

Lubetzky, Anat V; Price, Robert; McCoy, Sarah W

2016-07-01

Functional ankle instability is associated with decreased ankle muscle function. Compliant surfaces and eyes-closed training are commonly used for rehabilitation and prevention of ankle sprains. Brief Achilles tendon vibration is commonly used in the study of postural control. To test the level of activation of tibialis anterior (TIB) and fibularis longus (FIB), bilateral Achilles tendon vibration was applied for the middle 20 s in a series of 60-s trials, when 10 healthy young adults and 10 adults with history of repeated ankle sprains were standing bipedal: on floor, on memory foam, or on a Both Sides Up (BOSU) ball, with eyes open, and on floor and foam with eyes closed. Differences in Integrated surface electromyography (IEMG) of TIB and FIB were significant for both groups pre, during, and post vibration (Friedman Tests, p < 0.001 for all). In both groups, the highest IEMG for TIB was obtained during vibration when standing on foam with eyes closed, whereas the highest IEMG for FIB was obtained during vibration when standing on the BOSU. Bipedal stance on BOSU and brief Achilles tendon vibration may be a useful intervention when a session's goal is to facilitate lower leg muscles activation. Future research should explore training effects as well as the effect of FIB tendon vibration. Copyright © 2016 Elsevier Ltd. All rights reserved.

Vibrational dynamics of hydrogen-bonded complexes in solutions studied with ultrafast infrared pump-probe spectroscopy.

PubMed

Banno, Motohiro; Ohta, Kaoru; Yamaguchi, Sayuri; Hirai, Satori; Tominaga, Keisuke

2009-09-15

In aqueous solution, the basis of all living processes, hydrogen bonding exerts a powerful effect on chemical reactivity. The vibrational energy relaxation (VER) process in hydrogen-bonded complexes in solution is sensitive to the microscopic environment around the oscillator and to the geometrical configuration of the hydrogen-bonded complexes. In this Account, we describe the use of time-resolved infrared (IR) pump-probe spectroscopy to study the vibrational dynamics of (i) the carbonyl CO stretching modes in protic solvents and (ii) the OH stretching modes of phenol and carboxylic acid. In these cases, the carbonyl group acts as a hydrogen-bond acceptor, whereas the hydroxyl group acts as a hydrogen-bond donor. These vibrational modes have different properties depending on their respective chemical bonds, suggesting that hydrogen bonding may have different mechanisms and effects on the VER of the CO and OH modes than previously understood. The IR pump-probe signals of the CO stretching mode of 9-fluorenone and methyl acetate in alcohol, as well as that of acetic acid in water, include several components with different time constants. Quantum chemical calculations indicate that the dynamical components are the result of various hydrogen-bonded complexes that form between solute and solvent molecules. The acceleration of the VER is due to the increasing vibrational density of states caused by the formation of hydrogen bonds. The vibrational dynamics of the OH stretching mode in hydrogen-bonded complexes were studied in several systems. For phenol-base complexes, the decay time constant of the pump-probe signal decreases as the band peak of the IR absorption spectrum shifts to lower wavenumbers (the result of changing the proton acceptor). For phenol oligomers, the decay time constant of the pump-probe signal decreases as the probe wavenumber decreases. These observations show that the VER time strongly correlates with the strength of hydrogen bonding. This

Ultrafast dynamics of the photo-excited hemes b and cn in the cytochrome b6f complex.

PubMed

Agarwal, Rachna; Chauvet, Adrien A P

2017-01-25

The dynamics of hemes b and c n within the cytochrome b 6 f complex are investigated by means of ultrafast broad-band transient absorption spectroscopy. On the one hand, the data reveal that, subsequent to visible light excitation, part of the b hemes undergoes pulse-limited photo-oxidation, with the liberated electron supposedly being transferred to one of the adjacent aromatic amino acids. Photo-oxidation is followed by charge recombination in about 8.2 ps. Subsequent to charge recombination, heme b is promoted to a vibrationally excited ground state that relaxes in about 4.6 ps. On the other hand, heme c n undergoes ultrafast ground state recovery in about 140 fs. Interestingly, the data also show that, in contrast to previous beliefs, Chl a is involved in the photochemistry of hemes. Indeed, subsequent to heme excitation, Chl a bleaches and recovers to its ground state in 90 fs and 650 fs, respectively. Chl a bleaching allegedly corresponds to the formation of a short lived Chl a anion. Beyond the previously suggested structural role, this study provides unique evidence that Chl a is directly involved in the photochemistry of the hemes.

Vibration measurement by atomic force microscopy with laser readout

NASA Astrophysics Data System (ADS)

Snitka, Valentinas J.; Mizariene, Vida; Kalinauskas, Margiris; Lucinskas, Paulius

1998-06-01

Micromachined cantilever beams are widely used for different microengineering and nanotechnology actuators and sensors applications. The micromechanical cantilever tip-based data storage devices with reading real data at the rates exceeding 1Mbit/s have been demonstrated. The vibrational noise spectrum of a cantilever limits the data storage resolution. Therefore the possibility to measure the microvibrations and acoustic fields in different micromachined devices are of great interest. We describe a method to study a micromechanical cantilever and surface vibrations based on laser beam deflection measurements. The influence of piezoelectric plate vibrations and the tip- surface contact condition on the cantilever vibrations were investigated in the frequency range of 1-200 kHz. The experiments were performed using the measurement results. The V-shaped cantilevers exited by the normal vibrations due to the non-linearity at the tip-surface contact vibrates with a complex motion and has a lateral vibration mode coupled with normal vibration mode. The possibility to use laser deflection technique for the vibration measurements in micromachined structures with nano resolution is shown.

A new potential energy surface for vibration-vibration coupling in HF-HF collisions. Formulation and quantal scattering calculations

NASA Astrophysics Data System (ADS)

Schwenke, David W.; Truhlar, Donald G.

1988-04-01

We present new ab initio calculations of the HF-HF interaction potential for the case where both molecules are simultaneously displaced from their equilibrium internuclear distance. These and previous ab initio calculations are then fit to a new analytic representation which is designed to be efficient to evaluate and to provide an especially faithful account of the forces along the vibrational coordinates. We use the new potential for two sets of quantal scattering calculations for collisions in three dimensions with total angular momentum zero. First we test that the angular harmonic representation of the anisotropy is adequate by comparing quantal rigid rotator calculations to those carried out for potentials involving higher angular harmonics and for which the expansion in angular harmonics is systematically increased to convergence. Then we carry out large-scale quantal calculations of vibration-vibration energy transfer including the coupling of both sets of vibrational and rotational coordinates. These calculations indicate that significant rotational energy transfer accompanies the vibration-to-vibration energy transfer process.

Vibrational Mode-Specific Reaction of Methane with a Nickel Surface

NASA Astrophysics Data System (ADS)

Beck, Rainer

2004-03-01

The dissociation of methane on a nickel catalyst is a key step in steam reforming of natural gas for hydrogen production. Despite substantial effort in both experiment and theory, there is still no atomic scale description of this important gas-surface reaction. To elucidate its dynamics, we have performed quantum state resolved studies of vibrationally excited methane reacting on the Ni(100) surface using pulsed laser and molecular beam techniques. We observed up to a factor of 5 greater reaction probability for methane-d2 with two quanta of excitation in one C-H bond versus a nearly isoenergetic state with one quanta in each of two C-H bonds. The observed reactivities point to a transition state structure which has one of the C-H bonds significantly elongated. Our results also clearly exclude the possibility of statistical models correctly describing the mechanism of this process and emphasize the importance of full-dimensional calculations of the reaction dynamics.

Ultrafast Dynamics of Plasmon-Exciton Interaction of Ag Nanowire- Graphene Hybrids for Surface Catalytic Reactions

PubMed Central

Ding, Qianqian; Shi, Ying; Chen, Maodu; Li, Hui; Yang, Xianzhong; Qu, Yingqi; Liang, Wenjie; Sun, Mengtao

2016-01-01

Using the ultrafast pump-probe transient absorption spectroscopy, the femtosecond-resolved plasmon-exciton interaction of graphene-Ag nanowire hybrids is experimentally investigated, in the VIS-NIR region. The plasmonic lifetime of Ag nanowire is about 150 ± 7 femtosecond (fs). For a single layer of graphene, the fast dynamic process at 275 ± 77 fs is due to the excitation of graphene excitons, and the slow process at 1.4 ± 0.3 picosecond (ps) is due to the plasmonic hot electron interaction with phonons of graphene. For the graphene-Ag nanowire hybrids, the time scale of the plasmon-induced hot electron transferring to graphene is 534 ± 108 fs, and the metal plasmon enhanced graphene plasmon is about 3.2 ± 0.8 ps in the VIS region. The graphene-Ag nanowire hybrids can be used for plasmon-driven chemical reactions. This graphene-mediated surface-enhanced Raman scattering substrate significantly increases the probability and efficiency of surface catalytic reactions co-driven by graphene-Ag nanowire hybridization, in comparison with reactions individually driven by monolayer graphene or single Ag nanowire. This implies that the graphene-Ag nanowire hybrids can not only lead to a significant accumulation of high-density hot electrons, but also significantly increase the plasmon-to-electron conversion efficiency, due to strong plasmon-exciton coupling. PMID:27601199

A time-dependent order parameter for ultrafast photoinduced phase transitions.

PubMed

Beaud, P; Caviezel, A; Mariager, S O; Rettig, L; Ingold, G; Dornes, C; Huang, S-W; Johnson, J A; Radovic, M; Huber, T; Kubacka, T; Ferrer, A; Lemke, H T; Chollet, M; Zhu, D; Glownia, J M; Sikorski, M; Robert, A; Wadati, H; Nakamura, M; Kawasaki, M; Tokura, Y; Johnson, S L; Staub, U

2014-10-01

Strongly correlated electron systems often exhibit very strong interactions between structural and electronic degrees of freedom that lead to complex and interesting phase diagrams. For technological applications of these materials it is important to learn how to drive transitions from one phase to another. A key question here is the ultimate speed of such phase transitions, and to understand how a phase transition evolves in the time domain. Here we apply time-resolved X-ray diffraction to directly measure the changes in long-range order during ultrafast melting of the charge and orbitally ordered phase in a perovskite manganite. We find that although the actual change in crystal symmetry associated with this transition occurs over different timescales characteristic of the many electronic and vibrational coordinates of the system, the dynamics of the phase transformation can be well described using a single time-dependent 'order parameter' that depends exclusively on the electronic excitation.

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

NASA Astrophysics Data System (ADS)

Joo, Taiha

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

Reduced-vibration tube array

DOEpatents

Bruck, Gerald J.; Bartolomeo, Daniel R.

2004-07-20

A reduced-vibration tube array is disclosed. The array includes a plurality of tubes in a fixed arrangement and a plurality of damping members positioned within the tubes. The damping members include contoured interface regions characterized by bracing points that selectively contact the inner surface of an associated tube. Each interface region is sized and shaped in accordance with the associated tube, so that the damping member bracing points are spaced apart a vibration-reducing distance from the associated tube inner surfaces at equilibrium. During operation, mechanical interaction between the bracing points and the tube inner surfaces reduces vibration by a damage-reducing degree. In one embodiment, the interface regions are serpentine shaped. In another embodiment, the interface regions are helical in shape. The interface regions may be simultaneously helical and serpentine in shape. The damping members may be fixed within the associated tubes, and damping member may be customized several interference regions having attributes chosen in accordance with desired flow characteristics and associated tube properties.

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

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

Far-infrared vibration--rotation-tunneling spectroscopy of Ar--NH sub 3 : Intermolecular vibrations and effective angular potential energy surface

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

Schmuttenmaer, C.A.; Cohen, R.C.; Loeser, J.G.

Two new intermolecular vibration--rotation-tunneling (VRT) bands of Ar--NH{sub 3} have been measured using tunable far infrared laser spectroscopy. We have unambiguously assigned these and a previously measured FIR band (Gwo {ital et} {ital al}., Mol. Phys. {bold 71}, 453 (1990)) as {Pi}(1{sub 0}, {ital n}=0){l arrow}{Sigma}(0{sub 0}, {ital n}=0), {Sigma}(1{sub 0}, {ital n}=0){l arrow}{Sigma}(0{sub 0}, {ital n}=0), and {Sigma}(0{sub 0}, {ital n}=1){l arrow}{Sigma}(0{sub 0}, {ital n}=0). The three upper states of these are found to be strongly mixed by anisotropy and Coriolis effects. A simultaneous least squares fit of all transitions has yielded vibrational frequencies, rotational and centrifugal distortion constants,more » and a Coriolis parameter as well as quadrupole hyperfine coupling constants for the upper states. An effective angular potential energy surface for Ar--NH{sub 3} in its lowest stretching state has been determined from these data, after explicitly accounting for the effects of bend stretch interactions. Features of the surface include a global minimum at the near T-shaped configuration ({theta}=90{degree}), a 30 cm{sup {minus}1} to 60 cm{sup {minus}1} barrier to rotation at {theta}=180{degree} (or 0{degree}), and a very low barrier or possibly a secondary minimum at {theta}=0{degree} (or 180{degree}). Both attractive and repulsive interactions are shown to contribute significantly to the anisotropic forces in the complex. Comparison with {ital ab} {ital initio} calculations are presented.« less

Several new directions for ultrafast fiber lasers [Invited].

PubMed

Fu, Walter; Wright, Logan G; Sidorenko, Pavel; Backus, Sterling; Wise, Frank W

2018-04-16

Ultrafast fiber lasers have the potential to make applications of ultrashort pulses widespread - techniques not only for scientists, but also for doctors, manufacturing engineers, and more. Today, this potential is only realized in refractive surgery and some femtosecond micromachining. The existing market for ultrafast lasers remains dominated by solid-state lasers, primarily Ti:sapphire, due to their superior performance. Recent advances show routes to ultrafast fiber sources that provide performance and capabilities equal to, and in some cases beyond, those of Ti:sapphire, in compact, versatile, low-cost devices. In this paper, we discuss the prospects for future ultrafast fiber lasers built on new kinds of pulse generation that capitalize on nonlinear dynamics. We focus primarily on three promising directions: mode-locked oscillators that use nonlinearity to enhance performance; systems that use nonlinear pulse propagation to achieve ultrashort pulses without a mode-locked oscillator; and multimode fiber lasers that exploit nonlinearities in space and time to obtain unparalleled control over an electric field.

Ultrafast phosphate hydration dynamics in bulk H{sub 2}O

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

Costard, Rene, E-mail: costard@mbi-berlin.de; Tyborski, Tobias; Fingerhut, Benjamin P., E-mail: fingerhut@mbi-berlin.de

2015-06-07

Phosphate vibrations serve as local probes of hydrogen bonding and structural fluctuations of hydration shells around ions. Interactions of H{sub 2}PO{sub 4}{sup −} ions and their aqueous environment are studied combining femtosecond 2D infrared spectroscopy, ab-initio calculations, and hybrid quantum-classical molecular dynamics (MD) simulations. Two-dimensional infrared spectra of the symmetric (ν{sub S}(PO{sub 2}{sup −})) and asymmetric (ν{sub AS}(PO{sub 2}{sup −})) PO{sub 2}{sup −} stretching vibrations display nearly homogeneous lineshapes and pronounced anharmonic couplings between the two modes and with the δ(P-(OH){sub 2}) bending modes. The frequency-time correlation function derived from the 2D spectra consists of a predominant 50 fs decaymore » and a weak constant component accounting for a residual inhomogeneous broadening. MD simulations show that the fluctuating electric field of the aqueous environment induces strong fluctuations of the ν{sub S}(PO{sub 2}{sup −}) and ν{sub AS}(PO{sub 2}{sup −}) transition frequencies with larger frequency excursions for ν{sub AS}(PO{sub 2}{sup −}). The calculated frequency-time correlation function is in good agreement with the experiment. The ν(PO{sub 2}{sup −}) frequencies are mainly determined by polarization contributions induced by electrostatic phosphate-water interactions. H{sub 2}PO{sub 4}{sup −}/H{sub 2}O cluster calculations reveal substantial frequency shifts and mode mixing with increasing hydration. Predicted phosphate-water hydrogen bond (HB) lifetimes have values on the order of 10 ps, substantially longer than water-water HB lifetimes. The ultrafast phosphate-water interactions observed here are in marked contrast to hydration dynamics of phospholipids where a quasi-static inhomogeneous broadening of phosphate vibrations suggests minor structural fluctuations of interfacial water.« less

Multiphoton microscopy in every lab: the promise of ultrafast semiconductor disk lasers

NASA Astrophysics Data System (ADS)

Emaury, Florian; Voigt, Fabian F.; Bethge, Philipp; Waldburger, Dominik; Link, Sandro M.; Carta, Stefano; van der Bourg, Alexander; Helmchen, Fritjof; Keller, Ursula

2017-07-01

We use an ultrafast diode-pumped semiconductor disk laser (SDL) to demonstrate several applications in multiphoton microscopy. The ultrafast SDL is based on an optically pumped Vertical External Cavity Surface Emitting Laser (VECSEL) passively mode-locked with a semiconductor saturable absorber mirror (SESAM) and generates 170-fs pulses at a center wavelength of 1027 nm with a repetition rate of 1.63 GHz. We demonstrate the suitability of this laser for structural and functional multiphoton in vivo imaging in both Drosophila larvae and mice for a variety of fluorophores (including mKate2, tdTomato, Texas Red, OGB-1, and R-CaMP1.07) and for endogenous second-harmonic generation in muscle cell sarcomeres. We can demonstrate equivalent signal levels compared to a standard 80-MHz Ti:Sapphire laser when we increase the average power by a factor of 4.5 as predicted by theory. In addition, we compare the bleaching properties of both laser systems in fixed Drosophila larvae and find similar bleaching kinetics despite the large difference in pulse repetition rates. Our results highlight the great potential of ultrafast diode-pumped SDLs for creating a cost-efficient and compact alternative light source compared to standard Ti:Sapphire lasers for multiphoton imaging.

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.

Vibrational properties of the Au-(√{3 }×√{3 } )/Si(111) surface reconstruction

NASA Astrophysics Data System (ADS)

Halbig, B.; Liebhaber, M.; Bass, U.; Geurts, J.; Speiser, E.; Räthel, J.; Chandola, S.; Esser, N.; Krenz, M.; Neufeld, S.; Schmidt, W. G.; Sanna, S.

2018-01-01

The vibrational properties of the Au-induced (√{3 }×√{3 })R 30∘ reconstruction of the Si(111) surface are investigated by polarized surface Raman spectroscopy and density-functional theory. The Raman measurements are performed in situ at room temperature as well as 20 K, and they reveal the presence of vibrational eigenmodes in the spectral range from 20 to 450 cm-1. In particular, two peaks of E symmetry at 75 and 183 cm-1 dominate the spectra. No substantial difference between room- and low-temperature spectra is observed, suggesting that the system does not undergo a phase transition down to 20 K. First-principles calculations are performed based on the structural models discussed in the literature. The thermodynamically stable conjugate honeycomb-chained-trimer model (CHCT) [Surf. Sci. 275, L691 (1992), 10.1016/0039-6028(92)90785-5] leads to phonon eigenvalues compatible with the experimental observations in the investigated spectral range. On the basis of the phonon eigenfrequencies, symmetries, and Raman intensities, we assign the measured spectral features to the calculated phonon modes. The good agreement between measured and calculated modes provides a strong argument in favor of the CHCT model.

Process optimization for ultrasonic vibration assisted polishing of micro-structured surfaces on super hard material

NASA Astrophysics Data System (ADS)

Sun, Zhiyuan; Guo, Bing; Rao, Zhimin; Zhao, Qingliang

2014-08-01

In consideration of the excellent property of SiC, the ground micro-structured surface quality is hard to meet the requirement - consequently the ultrasonic vibration assisted polishing (UVAP) of micro-structures of molds is proposed in this paper. Through the orthogonal experiment, the parameters of UVAP of micro-structures were optimized. The experimental results show that, abrasive polishing process, the effect of the workpiece feed rate on the surface roughness (Ra), groove tip radius (R) and material removal rate (MRR) of micro-structures is significant. While, the UVAP, the most significant effect factor for Ra, R and MRR is the ultrasonic amplitude of the ultrasonic vibration. In addition, within the scope of the polishing process parameters selected by preliminary experiments, ultrasonic amplitude of 2.5μm, polishing force of 0.5N, workpiece feed rate of 5 mm·min-1, polishing wheel rotational speed of 50rpm, polishing time of 35min, abrasive size of 100nm and the polishing liquid concentration of 15% is the best technology of UVAP of micro-structures. Under the optimal parameters, the ground traces on the micro-structured surface were removed efficiently and the integrity of the edges of the micro-structure after grinding was maintained efficiently.

Full-Dimensional Quantum Calculations of Vibrational Levels of NH4(+) and Isotopomers on An Accurate Ab Initio Potential Energy Surface.

PubMed

Yu, Hua-Gen; Han, Huixian; Guo, Hua

2016-04-14

Vibrational energy levels of the ammonium cation (NH4(+)) and its deuterated isotopomers are calculated using a numerically exact kinetic energy operator on a recently developed nine-dimensional permutation invariant semiglobal potential energy surface fitted to a large number of high-level ab initio points. Like CH4, the vibrational levels of NH4(+) and ND4(+) exhibit a polyad structure, characterized by a collective quantum number P = 2(v1 + v3) + v2 + v4. The low-lying vibrational levels of all isotopomers are assigned and the agreement with available experimental data is better than 1 cm(-1).

Ultrafast dynamics of liquid water: Energy relaxation and transfer processes of the OH stretch and the HOH bend

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

Imoto, Sho; Xantheas, Sotiris S.; Saito, Shinji

2015-08-27

The vibrational energy relaxation and transfer processes of the OH stretching and the HOH bending vibrations in liquid water are investigated via the theoretical calculation of the pump-probe spectra obtained from non-equilibrium molecular dynamics simulations with the TTM3-F interaction potential. The excitation of the OH stretch induces an instantaneous response of the high frequency librational motions in the 600-1000 cm-1 range. In addition, the excess energy of the OH stretch of a water molecule quickly transfers to the OH stretches of molecules in its first hydration shell with a time constant of ~50 fs, followed by relaxation to the HOHmore » bends of the surrounding molecules with a time constant of 230 fs. The excitation of the HOH bend also results in the ultrafast excitation of the high frequency librational motions. The energy of the excited HOH bend of a water molecule decays, with a time constant of 200 fs, mainly to the relaxation of the HOH bends of its surrounding molecules. The energies of the HOH bends were found to transfer quickly to the intermolecular motions via the coupling with the high frequency librational motions. The excess energy of the OH stretch or the HOH bend relaxes to the high frequency intermolecular librational motions and eventually to the hot ground state with a time scale of ~1 ps via the coupling with the librational and translational motions. The energy relaxation and transfer processes were found to depend on the local hydrogen bonding network; the relaxations of the excess energy of the OH stretch and the HOH bend of four- and five-coordinated molecules are faster than those of a three-coordinated molecule due to the delocalization of the vibrational motions of the former (four- and five-coordinated molecules) compared to those of the later (three-coordinated molecules). The present results highlight the importance of the high frequency intermolecular librational modes in facilitating the ultrafast energy relaxation

Mechanism of vibrational energy dissipation of free OH groups at the air–water interface

PubMed Central

Hsieh, Cho-Shuen; Campen, R. Kramer; Okuno, Masanari; Backus, Ellen H. G.; Nagata, Yuki; Bonn, Mischa

2013-01-01

Interfaces of liquid water play a critical role in a wide variety of processes that occur in biology, a variety of technologies, and the environment. Many macroscopic observations clarify that the properties of liquid water interfaces significantly differ from those of the bulk liquid. In addition to interfacial molecular structure, knowledge of the rates and mechanisms of the relaxation of excess vibrational energy is indispensable to fully understand physical and chemical processes of water and aqueous solutions, such as chemical reaction rates and pathways, proton transfer, and hydrogen bond dynamics. Here we elucidate the rate and mechanism of vibrational energy dissipation of water molecules at the air–water interface using femtosecond two-color IR-pump/vibrational sum-frequency probe spectroscopy. Vibrational relaxation of nonhydrogen-bonded OH groups occurs at a subpicosecond timescale in a manner fundamentally different from hydrogen-bonded OH groups in bulk, through two competing mechanisms: intramolecular energy transfer and ultrafast reorientational motion that leads to free OH groups becoming hydrogen bonded. Both pathways effectively lead to the transfer of the excited vibrational modes from free to hydrogen-bonded OH groups, from which relaxation readily occurs. Of the overall relaxation rate of interfacial free OH groups at the air–H2O interface, two-thirds are accounted for by intramolecular energy transfer, whereas the remaining one-third is dominated by the reorientational motion. These findings not only shed light on vibrational energy dynamics of interfacial water, but also contribute to our understanding of the impact of structural and vibrational dynamics on the vibrational sum-frequency line shapes of aqueous interfaces. PMID:24191016

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

A sensitive and stable confocal Fabry-Pérot interferometer for surface ultrasonic vibration detection

NASA Astrophysics Data System (ADS)

Ding, Hong-sheng; Tong, Li-ge; Chen, Geng-hua

2001-08-01

A new confocal Fabry-Pérot interferometer (CFPI) has been constructed. By using both of the conjugate rays, the sensitivity of the system was doubled. Moreover, the negative feedback control loop of a single-chip microcomputer (MCS-51) was applied to stabilize the working point at an optimum position. The system has been used in detecting the piezoelectric ultrasonic vibration on the surface of an aluminium sample.

Modeling of induced seismicity and ground vibrations associated with geologic CO 2 storage, and assessing their effects on surface structures and human perception

DOE PAGES

Rutqvist, Jonny; Cappa, Frédéric; Rinaldi, Antonio P.; ...

2014-05-01

In this paper, we present model simulations of ground motions caused by CO 2 -injection-induced fault reactivation and analyze the results in terms of the potential for damage to ground surface structures and nuisance to the local human population. It is an integrated analysis from cause to consequence, including the whole chain of processes starting from earthquake inception in the subsurface, wave propagation toward the ground surface, and assessment of the consequences of ground vibration. For a small magnitude (M w =3) event at a hypocenter depth of about 1000m, we first used the simulated ground-motion wave train in anmore » inverse analysis to estimate source parameters (moment magnitude, rupture dimensions and stress drop), achieving good agreement and thereby verifying the modeling of the chain of processes from earthquake inception to ground vibration. We then analyzed the ground vibration results in terms of peak ground acceleration (PGA), peak ground velocity (PGV) and frequency content, with comparison to U.S. Geological Survey's instrumental intensity scales for earthquakes and the U.S. Bureau of Mines' vibration criteria for cosmetic damage to buildings, as well as human-perception vibration limits. Our results confirm the appropriateness of using PGV (rather than PGA) and frequency for the evaluation of potential ground-vibration effects on structures and humans from shallow injection-induced seismic events. For the considered synthetic M w =3 event, our analysis showed that the short duration, high frequency ground motion may not cause any significant damage to surface structures, but would certainly be felt by the local population.« less

Vibrational Spectroscopy on Photoexcited Dye-Sensitized Films via Pump-Degenerate Four-Wave Mixing.

PubMed

Abraham, Baxter; Fan, Hao; Galoppini, Elena; Gundlach, Lars

2018-03-01

Molecular sensitization of semiconductor films is an important technology for energy and environmental applications including solar energy conversion, photocatalytic hydrogen production, and water purification. Dye-sensitized films are also scientifically complex and interesting systems with a long history of research. In most applications, photoinduced heterogeneous electron transfer (HET) at the molecule/semiconductor interface is of critical importance, and while great progress has been made in understanding HET, many open questions remain. Of particular interest is the role of combined electronic and vibrational effects and coherence of the dye during HET. The ultrafast nature of the process, the rapid intramolecular vibrational energy redistribution, and vibrational cooling present complications in the study of vibronic coupling in HET. We present the application of a time domain vibrational spectroscopy-pump-degenerate four-wave mixing (pump-DFWM)-to dye-sensitized solid-state semiconductor films. Pump-DFWM can measure Raman-active vibrational modes that are triggered by excitation of the sample with an actinic pump pulse. Modifications to the instrument for solid-state samples and its application to an anatase TiO 2 film sensitized by a Zn-porphyrin dye are discussed. We show an effective combination of experimental techniques to overcome typical challenges in measuring solid-state samples with laser spectroscopy and observe molecular vibrations following HET in a picosecond time window. The cation spectrum of the dye shows modes that can be assigned to the linker group and a mode that is localized on the Zn-phorphyrin chromophore and that is connected to photoexcitation.

Good Vibrations

NASA Technical Reports Server (NTRS)

2001-01-01

A Small Business Innovation Research (SBIR) sponsorship from NASA's Dryden Flight Research Center, assisted MetroLaser, of Irvine, California, in the development of a self-aligned laser vibrometer system. VibroMet, capable of measuring surface vibrations in a variety of industries, provides information on the structural integrity and acoustical characteristics of manufactured products. This low-cost, easy-to-use sensor performs vibration measurement from distances of up to three meters without the need for adjustment. The laser beam is simply pointed at the target and the system then uses a compact laser diode to illuminate the surface and to subsequently analyze the reflected light. The motion of the surface results in a Doppler shift that is measured with very high precision. VibroMet is considered one of the many behind-the-scenes tools that can be relied on to assure the quality, reliability and safety of everything from airplane panels to disk brakes

Giant ultrafast Kerr effect in superconductors

NASA Astrophysics Data System (ADS)

Robson, Charles W.; Fraser, Kieran A.; Biancalana, Fabio

2017-06-01

We study the ultrafast Kerr effect and high-harmonic generation in superconductors by formulating a model for a time-varying electromagnetic pulse normally incident on a thin-film superconductor. It is found that superconductors exhibit exceptionally large χ(3 ) due to the progressive destruction of Cooper pairs, and display high-harmonic generation at low incident intensities, and the highest nonlinear susceptibility of all known materials in the THz regime. Our theory opens up avenues for accessible analytical and numerical studies of the ultrafast dynamics of superconductors.

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

Surface recombination of oxygen atoms in O2 plasma at increased pressure: II. Vibrational temperature and surface production of ozone

NASA Astrophysics Data System (ADS)

Lopaev, D. V.; Malykhin, E. M.; Zyryanov, S. M.

2011-01-01

Ozone production in an oxygen glow discharge in a quartz tube was studied in the pressure range of 10-50 Torr. The O3 density distribution along the tube diameter was measured by UV absorption spectroscopy, and ozone vibrational temperature TV was found comparing the calculated ab initio absorption spectra with the experimental ones. It has been shown that the O3 production mainly occurs on a tube surface whereas ozone is lost in the tube centre where in contrast the electron and oxygen atom densities are maximal. Two models were used to analyse the obtained results. The first one is a kinetic 1D model for the processes occurring near the tube walls with the participation of the main particles: O(3P), O2, O2(1Δg) and O3 molecules in different vibrational states. The agreement of O3 and O(3P) density profiles and TV calculated in the model with observed ones was reached by varying the single model parameter—ozone production probability (\\gamma_{O_{3}}) on the quartz tube surface on the assumption that O3 production occurs mainly in the surface recombination of physisorbed O(3P) and O2. The phenomenological model of the surface processes with the participation of oxygen atoms and molecules including singlet oxygen molecules was also considered to analyse \\gamma_{O_{3}} data obtained in the kinetic model. A good agreement between the experimental data and the data of both models—the kinetic 1D model and the phenomenological surface model—was obtained in the full range of the studied conditions that allowed consideration of the ozone surface production mechanism in more detail. The important role of singlet oxygen in ozone surface production was shown. The O3 surface production rate directly depends on the density of physisorbed oxygen atoms and molecules and can be high with increasing pressure and energy inputted into plasma while simultaneously keeping the surface temperature low enough. Using the special discharge cell design, such an approach opens up the

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

Direct Characterization of Ultrafast Energy-Time Entangled Photon Pairs.

PubMed

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

2018-02-02

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

Full-dimensional quantum calculations of vibrational levels of NH 4 + and isotopomers on an accurate ab initio potential energy surface

DOE PAGES

Hua -Gen Yu; Han, Huixian; Guo, Hua

2016-03-29

Vibrational energy levels of the ammonium cation (NH 4 +) and its deuterated isotopomers are calculated using a numerically exact kinetic energy operator on a recently developed nine-dimensional permutation invariant semiglobal potential energy surface fitted to a large number of high-level ab initio points. Like CH4, the vibrational levels of NH 4 + and ND 4 + exhibit a polyad structure, characterized by a collective quantum number P = 2(v 1 + v 3) + v 2 + v 4. As a result, the low-lying vibrational levels of all isotopomers are assigned and the agreement with available experimental data ismore » better than 1 cm –1.« less

Ultrafast Ultrasound Imaging With Cascaded Dual-Polarity Waves.

PubMed

Zhang, Yang; Guo, Yuexin; Lee, Wei-Ning

2018-04-01

Ultrafast ultrasound imaging using plane or diverging waves, instead of focused beams, has advanced greatly the development of novel ultrasound imaging methods for evaluating tissue functions beyond anatomical information. However, the sonographic signal-to-noise ratio (SNR) of ultrafast imaging remains limited due to the lack of transmission focusing, and thus insufficient acoustic energy delivery. We hereby propose a new ultrafast ultrasound imaging methodology with cascaded dual-polarity waves (CDWs), which consists of a pulse train with positive and negative polarities. A new coding scheme and a corresponding linear decoding process were thereby designed to obtain the recovered signals with increased amplitude, thus increasing the SNR without sacrificing the frame rate. The newly designed CDW ultrafast ultrasound imaging technique achieved higher quality B-mode images than coherent plane-wave compounding (CPWC) and multiplane wave (MW) imaging in a calibration phantom, ex vivo pork belly, and in vivo human back muscle. CDW imaging shows a significant improvement in the SNR (10.71 dB versus CPWC and 7.62 dB versus MW), penetration depth (36.94% versus CPWC and 35.14% versus MW), and contrast ratio in deep regions (5.97 dB versus CPWC and 5.05 dB versus MW) without compromising other image quality metrics, such as spatial resolution and frame rate. The enhanced image qualities and ultrafast frame rates offered by CDW imaging beget great potential for various novel imaging applications.

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

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

Excitation laser energy dependence of surface-enhanced fluorescence showing plasmon-induced ultrafast electronic dynamics in dye molecules

NASA Astrophysics Data System (ADS)

Itoh, Tamitake; Yamamoto, Yuko S.; Tamaru, Hiroharu; Biju, Vasudevanpillai; Murase, Norio; Ozaki, Yukihiro

2013-06-01

We find unique properties accompanying surface-enhanced fluorescence (SEF) from dye molecules adsorbed on Ag nanoparticle aggregates, which generate surface-enhanced Raman scattering. The properties are observed in excitation laser energy dependence of SEF after excluding plasmonic spectral modulation in SEF. The unique properties are large blue shifts of fluorescence spectra, deviation of ratios between anti-Stokes SEF intensity and Stokes from those of normal fluorescence, super-broadening of Stokes spectra, and returning to original fluorescence by lower energy excitation. We elucidate that these properties are induced by electromagnetic enhancement of radiative decay rates exceeding the vibrational relaxation rates within an electronic excited state, which suggests that molecular electronic dynamics in strong plasmonic fields can be largely deviated from that in free space.

Salt Effects on Surface Structures of Polyelectrolyte Multilayers (PEMs) Investigated by Vibrational Sum Frequency Generation (SFG) Spectroscopy.

PubMed

Ge, Aimin; Matsusaki, Michiya; Qiao, Lin; Akashi, Mitsuru; Ye, Shen

2016-04-26

Sum frequency generation (SFG) vibrational spectroscopy was employed to investigate the surface structures of polyelectrolyte multilayers (PEMs) constructed by sequentially alternating adsorption of poly(diallyldimethylammonium chloride) (PDDA) and poly(styrenesulfonate) (PSS). It was found that the surface structures and surface charge density of the as-deposited PEMs of PDDA/PSS significantly depend on the concentration of sodium chloride (NaCl) present in the polyelectrolyte solutions. Furthermore, it was found that the surface structure of the as-deposited PEMs is in a metastable state and will reach the equilibrium state by diffusion of the polyelectrolyte chain after an aging process, resulting in a polyelectrolyte mixture on the PEM surfaces.

Electronic and structural response of nanomaterials to ultrafast and ultraintense laser pulses.

PubMed

Jiang, Chen-Wei; Zhou, Xiang; Lin, Zhibin; Xie, Rui-Hua; Li, Fu-Li; Allen, Roland E

2014-02-01

The interaction of materials with ultrafast and ultraintense laser pulses is a current frontier of science both experimentally and theoretically. In this review, we briefly discuss some recent theoretical studies by the present authors with our method of semiclassical electron-radiation-ion dynamics (SERID). In particular, Zhou et al. and Jiang et al. respectively, determined the optimal duration and optimal timing for a series of femtosecond scale laser pulses to excite a specific vibrational mode in a general chemical system. A set of such modes can be used as a "fingerprint" for characterizing a particular molecule or a complex in a solid. One can therefore envision many applications, ranging from fundamental studies to detection of chemical or biological agents. Allen et al. proved that dimers are preferentially emitted during photofragmentation of C60 under an ultrafast and ultraintense laser pulse. For interactions between laser pulses and semiconductors, e.g., GaAs, Si and InSb, besides experimentally accessible optical properties--epsilon(omega) and chi(2)-Allen et al. offered many other indicators to confirm the nonthermal nature of structural changes driven by electronic excitations and occurring during the first few hundred femtoseconds. Lin et al. found that, after the application of a femtosecond laser pulse, excited electrons in materials automatically equilibrate to a Fermi-Dirac distribution within roughly 100 fs, solely because of their coupling to the nuclear motion, even though the resulting electronic temperature is one to two orders of magnitude higher than the kinetic temperature defined by the nuclear motion.

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.

Ultrafast dynamics of differently aligned COOH-DTE-BODIPY conjugates linked to the surface of TiO2

NASA Astrophysics Data System (ADS)

Schweighöfer, Felix; Yüce, Imanuel; Dworak, Lars; Guo, Peng; Zastrow, Marc; Mayer, Kerstin; Barta, Christoph; Liebmann, Diana; Ziebart, Nandor; Rück-Braun, Karola; Wachtveitl, Josef

2018-02-01

The photoinduced dynamics of two DTE-BODIPY conjugates A, B with carboxylic acid anchoring groups coupled to the surface of TiO2 were studied by ultrafast transient absorption spectroscopy. For compound A, with an orthogonal orientation of the BODIPY chromophore and the photoswitchable DTE unit, a charge separated state could not be reliably detected. Nevertheless, besides the energy transfer from the BODIPY to the ring-closed DTE-c, indications for an electron transfer reaction were found by analyzing fluorescence quenching on TiO2 in steady state fluorescence measurements. For compound B with a parallel orientation of chromophore and photoswitch, a charge separated state was conclusively identified for the coupled dyad (TiO2) via the observation of a positive absorption signal (at λ pr  >  610 nm) at later delay times. An electron transfer rate of 7  ×  1010 s-1 can be extracted, indicating slower processes in the dyads in comparison to previously published electron transfer reactions of DTE compounds coupled to TiO2.

Ultrafast dynamics of differently aligned COOH-DTE-BODIPY conjugates linked to the surface of TiO2.

PubMed

Schweighöfer, Felix; Yüce, Imanuel; Dworak, Lars; Guo, Peng; Zastrow, Marc; Mayer, Kerstin; Barta, Christoph; Liebmann, Diana; Ziebart, Nandor; Rück-Braun, Karola; Wachtveitl, Josef

2018-01-05

The photoinduced dynamics of two DTE-BODIPY conjugates A, B with carboxylic acid anchoring groups coupled to the surface of TiO 2 were studied by ultrafast transient absorption spectroscopy. For compound A, with an orthogonal orientation of the BODIPY chromophore and the photoswitchable DTE unit, a charge separated state could not be reliably detected. Nevertheless, besides the energy transfer from the BODIPY to the ring-closed DTE-c, indications for an electron transfer reaction were found by analyzing fluorescence quenching on TiO 2 in steady state fluorescence measurements. For compound B with a parallel orientation of chromophore and photoswitch, a charge separated state was conclusively identified for the coupled dyad (TiO 2 ) via the observation of a positive absorption signal (at λ pr   >  610 nm) at later delay times. An electron transfer rate of 7  ×  10 10 s -1 can be extracted, indicating slower processes in the dyads in comparison to previously published electron transfer reactions of DTE compounds coupled to TiO 2 .

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.

Ultrafast vibrational spectroscopy (2D-IR) of CO{sub 2} in ionic liquids: Carbon capture from carbon dioxide’s point of view

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

Brinzer, Thomas; Berquist, Eric J.; Ren, Zhe

2015-06-07

The CO{sub 2}ν{sub 3} asymmetric stretching mode is established as a vibrational chromophore for ultrafast two-dimensional infrared (2D-IR) spectroscopic studies of local structure and dynamics in ionic liquids, which are of interest for carbon capture applications. CO{sub 2} is dissolved in a series of 1-butyl-3-methylimidazolium-based ionic liquids ([C{sub 4}C{sub 1}im][X], where [X]{sup −} is the anion from the series hexafluorophosphate (PF{sub 6}{sup −}), tetrafluoroborate (BF{sub 4}{sup −}), bis-(trifluoromethyl)sulfonylimide (Tf{sub 2}N{sup −}), triflate (TfO{sup −}), trifluoroacetate (TFA{sup −}), dicyanamide (DCA{sup −}), and thiocyanate (SCN{sup −})). In the ionic liquids studied, the ν{sub 3} center frequency is sensitive to the local solvationmore » environment and reports on the timescales for local structural relaxation. Density functional theory calculations predict charge transfer from the anion to the CO{sub 2} and from CO{sub 2} to the cation. The charge transfer drives geometrical distortion of CO{sub 2}, which in turn changes the ν{sub 3} frequency. The observed structural relaxation timescales vary by up to an order of magnitude between ionic liquids. Shoulders in the 2D-IR spectra arise from anharmonic coupling of the ν{sub 2} and ν{sub 3} normal modes of CO{sub 2}. Thermal fluctuations in the ν{sub 2} population stochastically modulate the ν{sub 3} frequency and generate dynamic cross-peaks. These timescales are attributed to the breakup of ion cages that create a well-defined local environment for CO{sub 2}. The results suggest that the picosecond dynamics of CO{sub 2} are gated by local diffusion of anions and cations.« less

Structural sensitivity of Csbnd H vibrational band in methyl benzoate

NASA Astrophysics Data System (ADS)

Roy, Susmita; Maiti, Kiran Sankar

2018-05-01

The Csbnd H vibrational bands of methyl benzoate are studied to understand its coupling pattern with other vibrational bands of the biological molecule. This will facilitate to understand the biological structure and dynamics in spectroscopic as well as in microscopic study. Due to the congested spectroscopic pattern, near degeneracy, and strong anharmonicity of the Csbnd H stretch vibrations, assignment of the Csbnd H vibrational frequencies are often misleading. Anharmonic vibrational frequency calculation with multidimensional potential energy surface interprets the Csbnd H vibrational spectra more accurately. In this article we have presented the importance of multidimensional potential energy surface in anharmonic vibrational frequency calculation and discuss the unexpected red shift of asymmetric Csbnd H stretch vibration of methyl group. The Csbnd D stretch vibrational band which is splitted to double peaks due to the Fermi resonance is also discussed here.

Ultrafast electron and energy transfer in dye-sensitized iron oxide and oxyhydroxide nanoparticles.

PubMed

Gilbert, Benjamin; Katz, Jordan E; Huse, Nils; Zhang, Xiaoyi; Frandsen, Cathrine; Falcone, Roger W; Waychunas, Glenn A

2013-10-28

An emerging area in chemical science is the study of solid-phase redox reactions using ultrafast time-resolved spectroscopy. We have used molecules of the photoactive dye 2',7'-dichlorofluorescein (DCF) anchored to the surface of iron(III) oxide nanoparticles to create iron(II) surface atoms via photo-initiated interfacial electron transfer. This approach enables time-resolved study of the fate and mobility of electrons within the solid phase. However, complete analysis of the ultrafast processes following dye photoexcitation of the sensitized iron(III) oxide nanoparticles has not been reported. We addressed this topic by performing femtosecond transient absorption (TA) measurements of aqueous suspensions of uncoated and DCF-sensitized iron oxide and oxyhydroxide nanoparticles, and an aqueous iron(III)-dye complex. Following light absorption, excited state relaxation times of the dye of 115-310 fs were found for all samples. Comparison between TA dynamics on uncoated and dye-sensitized hematite nanoparticles revealed the dye de-excitation pathway to consist of a competition between electron and energy transfer to the nanoparticles. We analyzed the TA data for hematite nanoparticles using a four-state model of the dye-sensitized system, finding electron and energy transfer to occur on the same ultrafast timescale. The interfacial electron transfer rates for iron oxides are very close to those previously reported for DCF-sensitized titanium dioxide (for which dye-oxide energy transfer is energetically forbidden) even though the acceptor states are different. Comparison of the alignment of the excited states of the dye and the unoccupied states of these oxides showed that the dye injects into acceptor states of different symmetry (Ti t2gvs. Fe eg).

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.

The influence of the fault zone width on land surface vibrations after the high-energy tremor in the "Rydułtowy-Anna" hard coal mine

NASA Astrophysics Data System (ADS)

Pilecka, Elżbieta; Szwarkowski, Dariusz

2018-04-01

In the article, a numerical analysis of the impact of the width of the fault zone on land surface tremors on the area of the "Rydułtowy - Anna" hard coal mine was performed. The analysis covered the dynamic impact of the actual seismic wave after the high-energy tremor of 7 June 2013. Vibrations on the land surface are a measure of the mining damage risk. It is particularly the horizontal components of land vibrations that are dangerous to buildings which is reflected in the Mining Scales of Intensity (GSI) of vibrations. The run of a seismic wave in the rock mass from the hypocenter to the area's surface depends on the lithology of the area and the presence of fault zones. The rock mass network cut by faults of various widths influences the amplitude of tremor reaching the area's surface. The analysis of the impact of the width of the fault zone was done for three alternatives.

Vibrational Spectroscopy and Astrobiology

NASA Technical Reports Server (NTRS)

Chaban, Galina M.; Kwak, D. (Technical Monitor)

2001-01-01

Role of vibrational spectroscopy in solving problems related to astrobiology will be discussed. Vibrational (infrared) spectroscopy is a very sensitive tool for identifying molecules. Theoretical approach used in this work is based on direct computation of anharmonic vibrational frequencies and intensities from electronic structure codes. One of the applications of this computational technique is possible identification of biological building blocks (amino acids, small peptides, DNA bases) in the interstellar medium (ISM). Identifying small biological molecules in the ISM is very important from the point of view of origin of life. Hybrid (quantum mechanics/molecular mechanics) theoretical techniques will be discussed that may allow to obtain accurate vibrational spectra of biomolecular building blocks and to create a database of spectroscopic signatures that can assist observations of these molecules in space. Another application of the direct computational spectroscopy technique is to help to design and analyze experimental observations of ice surfaces of one of the Jupiter's moons, Europa, that possibly contains hydrated salts. The presence of hydrated salts on the surface can be an indication of a subsurface ocean and the possible existence of life forms inhabiting such an ocean.

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

Large-area tungsten disulfide for ultrafast photonics.

PubMed

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

2017-02-02

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

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.

Feed-forward motor control of ultrafast, ballistic movements.

PubMed

Kagaya, K; Patek, S N

2016-02-01

To circumvent the limits of muscle, ultrafast movements achieve high power through the use of springs and latches. The time scale of these movements is too short for control through typical neuromuscular mechanisms, thus ultrafast movements are either invariant or controlled prior to movement. We tested whether mantis shrimp (Stomatopoda: Neogonodactylus bredini) vary their ultrafast smashing strikes and, if so, how this control is achieved prior to movement. We collected high-speed images of strike mechanics and electromyograms of the extensor and flexor muscles that control spring compression and latch release. During spring compression, lateral extensor and flexor units were co-activated. The strike initiated several milliseconds after the flexor units ceased, suggesting that flexor activity prevents spring release and determines the timing of strike initiation. We used linear mixed models and Akaike's information criterion to serially evaluate multiple hypotheses for control mechanisms. We found that variation in spring compression and strike angular velocity were statistically explained by spike activity of the extensor muscle. The results show that mantis shrimp can generate kinematically variable strikes and that their kinematics can be changed through adjustments to motor activity prior to the movement, thus supporting an upstream, central-nervous-system-based control of ultrafast movement. Based on these and other findings, we present a shishiodoshi model that illustrates alternative models of control in biological ballistic systems. The discovery of feed-forward control in mantis shrimp sets the stage for the assessment of targets, strategic variation in kinematics and the role of learning in ultrafast animals. © 2016. Published by The Company of Biologists Ltd.

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

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.

SVMs for Vibration-Based Terrain Classification

NASA Astrophysics Data System (ADS)

Weiss, Christian; Stark, Matthias; Zell, Andreas

When an outdoor mobile robot traverses different types of ground surfaces, different types of vibrations are induced in the body of the robot. These vibrations can be used to learn a discrimination between different surfaces and to classify the current terrain. Recently, we presented a method that uses Support Vector Machines for classification, and we showed results on data collected with a hand-pulled cart. In this paper, we show that our approach also works well on an outdoor robot. Furthermore, we more closely investigate in which direction the vibration should be measured. Finally, we present a simple but effective method to improve the classification by combining measurements taken in multiple directions.

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 magnetization reversal by picosecond electrical pulses

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

Yang, Yang; Wilson, Richard B.; Gorchon, Jon

The field of spintronics involves the study of both spin and charge transport in solid-state devices. Ultrafast magnetism involves the use of femtosecond laser pulses to manipulate magnetic order on subpicosecond time scales. Here, we unite these phenomena by using picosecond charge current pulses to rapidly excite conduction electrons in magnetic metals. We observe deterministic, repeatable ultrafast reversal of the magnetization of a GdFeCo thin film with a single sub–10-ps electrical pulse. The magnetization reverses in ~10 ps, which is more than one order of magnitude faster than any other electrically controlled magnetic switching, and demonstrates a fundamentally new electricalmore » switching mechanism that does not require spin-polarized currents or spin-transfer/orbit torques. The energy density required for switching is low, projecting to only 4 fJ needed to switch a (20 nm) 3 cell. This discovery introduces a new field of research into ultrafast charge current–driven spintronic phenomena and devices.« less

Ultrafast magnetization reversal by picosecond electrical pulses

DOE PAGES

Yang, Yang; Wilson, Richard B.; Gorchon, Jon; ...

2017-11-03

The field of spintronics involves the study of both spin and charge transport in solid-state devices. Ultrafast magnetism involves the use of femtosecond laser pulses to manipulate magnetic order on subpicosecond time scales. Here, we unite these phenomena by using picosecond charge current pulses to rapidly excite conduction electrons in magnetic metals. We observe deterministic, repeatable ultrafast reversal of the magnetization of a GdFeCo thin film with a single sub–10-ps electrical pulse. The magnetization reverses in ~10 ps, which is more than one order of magnitude faster than any other electrically controlled magnetic switching, and demonstrates a fundamentally new electricalmore » switching mechanism that does not require spin-polarized currents or spin-transfer/orbit torques. The energy density required for switching is low, projecting to only 4 fJ needed to switch a (20 nm) 3 cell. This discovery introduces a new field of research into ultrafast charge current–driven spintronic phenomena and devices.« less

Inelastic vibrational bulk and surface losses of swift electrons in ionic nanostructures

NASA Astrophysics Data System (ADS)

Hohenester, Ulrich; Trügler, Andreas; Batson, Philip E.; Lagos, Maureen J.

2018-04-01

In a recent paper [Lagos et al., Nature (London) 543, 533 (2017), 10.1038/nature21699] we have used electron energy loss spectroscopy with sub-10 meV energy and atomic spatial resolution to map optical and acoustic, bulk and surface vibrational modes in magnesium oxide nanocubes. We found that a local dielectric description works well for the simulation of aloof geometries, similar to related work for surface plasmons and surface plasmon polaritons, while for intersecting geometries such a description fails to reproduce the rich spectral features associated with excitation of bulk acoustic and optical phonons. To account for scatterings with a finite momentum exchange, in this paper we investigate molecular and lattice dynamics simulations of bulk losses in magnesium-oxide nanocubes using a rigid-ion description and investigate the loss spectra for intersecting electron beams. From our analysis we can evaluate the capability of electron energy loss spectroscopy for the investigation of phonon modes at the nanoscale, and we discuss shortcomings of our simplified approach as well as directions for future investigations.

Vibration detecting apparatus for multi-rotor rotary piston engines

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

Fujimoto, Y.; Sasaki, H.; Karimata, Y.

1987-04-28

A multi-rotor rotary piston engine is described comprising rotor housings each having an inner wall surface of a two-lobe trochoidal form, an intermediate housing having opposite side surfaces and located between two adjacent ones of the rotor housings, a pair of side housings attached to outer surfaces of outermost rotor housings, rotors which are disposed in respective ones of the rotor housings and carried by an eccentric shaft, adjacent rotors each having a side surface adapted for sliding engagement with the side surfaces of the intermediate housing, vibration detecting means mounted on the intermediate housing for detecting engine vibrations, themore » vibration detecting means being oriented so that it has a sensitivity in the direction substantially perpendicular to the side surface of the intermediate housing.« less

Interfacial instabilities in vibrated fluids

NASA Astrophysics Data System (ADS)

Porter, Jeff; Laverón-Simavilla, Ana; Tinao Perez-Miravete, Ignacio; Fernandez Fraile, Jose Javier

2016-07-01

Vibrations induce a range of different interfacial phenomena in fluid systems depending on the frequency and orientation of the forcing. With gravity, (large) interfaces are approximately flat and there is a qualitative difference between vertical and horizontal forcing. Sufficient vertical forcing produces subharmonic standing waves (Faraday waves) that extend over the whole interface. Horizontal forcing can excite both localized and extended interfacial phenomena. The vibrating solid boundaries act as wavemakers to excite traveling waves (or sloshing modes at low frequencies) but they also drive evanescent bulk modes whose oscillatory pressure gradient can parametrically excite subharmonic surface waves like cross-waves. Depending on the magnitude of the damping and the aspect ratio of the container, these locally generated surfaces waves may interact in the interior resulting in temporal modulation and other complex dynamics. In the case where the interface separates two fluids of different density in, for example, a rectangular container, the mass transfer due to vertical motion near the endwalls requires a counterflow in the interior region that can lead to a Kelvin-Helmholtz type instability and a ``frozen wave" pattern. In microgravity, the dominance of surface forces favors non-flat equilibrium configurations and the distinction between vertical and horizontal applied forcing can be lost. Hysteresis and multiplicity of solutions are more common, especially in non-wetting systems where disconnected (partial) volumes of fluid can be established. Furthermore, the vibrational field contributes a dynamic pressure term that competes with surface tension to select the (time averaged) shape of the surface. These new (quasi-static) surface configurations, known as vibroequilibria, can differ substantially from the hydrostatic state. There is a tendency for the interface to orient perpendicular to the vibrational axis and, in some cases, a bulge or cavity is induced

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.

Ground test for vibration control demonstrator

NASA Astrophysics Data System (ADS)

Meyer, C.; Prodigue, J.; Broux, G.; Cantinaud, O.; Poussot-Vassal, C.

2016-09-01

In the objective of maximizing comfort in Falcon jets, Dassault Aviation is developing an innovative vibration control technology. Vibrations of the structure are measured at several locations and sent to a dedicated high performance vibration control computer. Control laws are implemented in this computer to analyse the vibrations in real time, and then elaborate orders sent to the existing control surfaces to counteract vibrations. After detailing the technology principles, this paper focuses on the vibration control ground demonstration that was performed by Dassault Aviation in May 2015 on Falcon 7X business jet. The goal of this test was to attenuate vibrations resulting from fixed forced excitation delivered by shakers. The ground test demonstrated the capability to implement an efficient closed-loop vibration control with a significant vibration level reduction and validated the vibration control law design methodology. This successful ground test was a prerequisite before the flight test demonstration that is now being prepared. This study has been partly supported by the JTI CleanSky SFWA-ITD.

Hydrogen Bond Lifetimes and Energetics for Solute-Solvent Complexes Studied with 2D-IR Vibrational Echo Spectroscopy

PubMed Central

Zheng, Junrong; Fayer, Michael D.

2008-01-01

Weak π hydrogen bonded solute-solvent complexes are studied with ultrafast two dimensional infrared (2D-IR) vibrational echo chemical exchange spectroscopy, temperature dependent IR absorption spectroscopy, and density functional theory calculations. Eight solute-solvent complexes composed of a number of phenol derivatives and various benzene derivatives are investigated. The complexes are formed between the phenol derivative (solute) in a mixed solvent of the benzene derivative and CCl4. The time dependence of the 2D-IR vibrational echo spectra of the phenol hydroxyl stretch is used to directly determine the dissociation and formation rates of the hydrogen bonded complexes. The dissociation rates of the weak hydrogen bonds are found to be strongly correlated with their formation enthalpies. The correlation can be described with an equation similar to the Arrhenius equation. The results are discussed in terms of transition state theory. PMID:17373792

Practical Design and Applications of Ultrafast Semiconductor Disk Lasers

NASA Astrophysics Data System (ADS)

Baker, Caleb W.

Vertical External Cavity Surface Emitting Lasers (VECSELs) have become well established in recent years for their design flexibility and promising power scalability. Recent efforts in VECSEL development have focused heavily on expanding the medium into the ultrafast regime of modelocked operation. Presented in this thesis is a detailed discussion regarding the development of ultrafast VECSEL devices. Achievements in continuous wave (CW) operation will be highlighted, followed by several chapters detailing the engineering challenges and design solutions which enable modelocked operation of VECSELs in the ultrafast regime, including the design of the saturable absorbers used to enforce modelocking, management of the net group delay dispersion (GDD) inside the cavity, and the design of the active region to support pulse durations on the order of 100 fs. Work involving specific applications - VECSELs emitting on multiple wavelengths simultaneously and the use of VECSEL seed oscillators for amplification and spectral broadening - will also be presented. Key experimental results will include a novel multi-fold cavity design that produced record-setting peak powers of 6.3 kW from a modelocked VECSEL, an octave-spanning supercontinuum with an average power of 2 W generated using a VECSEL seed and a 2-stage Yb fiber amplifier, and two separate experiments where a VECSEL was made to emit on multiple wavelengths simultaneously in modelocked and highly stable CW operation, respectively. Further, many diagnostic and characterization measurements will be presented, most notably the in-situ probing of a VECSEL gain medium during stable modelocked operation with temporal resolution on the order of 100 fs, but also including characterization of the relaxation rates in different saturable absorber designs and the effectiveness of different methods for managing the net GDD of a device.

Materials Properties and Solvated Electron Dynamics of Isolated Nanoparticles and Nanodroplets Probed with Ultrafast Extreme Ultraviolet Beams.

PubMed

Ellis, Jennifer L; Hickstein, Daniel D; Xiong, Wei; Dollar, Franklin; Palm, Brett B; Keister, K Ellen; Dorney, Kevin M; Ding, Chengyuan; Fan, Tingting; Wilker, Molly B; Schnitzenbaumer, Kyle J; Dukovic, Gordana; Jimenez, Jose L; Kapteyn, Henry C; Murnane, Margaret M

2016-02-18

We present ultrafast photoemission measurements of isolated nanoparticles in vacuum using extreme ultraviolet (EUV) light produced through high harmonic generation. Surface-selective static EUV photoemission measurements were performed on nanoparticles with a wide array of compositions, ranging from ionic crystals to nanodroplets of organic material. We find that the total photoelectron yield varies greatly with nanoparticle composition and provides insight into material properties such as the electron mean free path and effective mass. Additionally, we conduct time-resolved photoelectron yield measurements of isolated oleylamine nanodroplets, observing that EUV photons can create solvated electrons in liquid nanodroplets. Using photoemission from a time-delayed 790 nm pulse, we observe that a solvated electron is produced in an excited state and subsequently relaxes to its ground state with a lifetime of 151 ± 31 fs. This work demonstrates that femotosecond EUV photoemission is a versatile surface-sensitive probe of the properties and ultrafast dynamics of isolated nanoparticles.

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).

Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes

DOE PAGES

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

2016-02-15

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

Rational material design for ultrafast rechargeable lithium-ion batteries.

PubMed

Tang, Yuxin; Zhang, Yanyan; Li, Wenlong; Ma, Bing; Chen, Xiaodong

2015-10-07

Rechargeable lithium-ion batteries (LIBs) are important electrochemical energy storage devices for consumer electronics and emerging electrical/hybrid vehicles. However, one of the formidable challenges is to develop ultrafast charging LIBs with the rate capability at least one order of magnitude (>10 C) higher than that of the currently commercialized LIBs. This tutorial review presents the state-of-the-art developments in ultrafast charging LIBs by the rational design of materials. First of all, fundamental electrochemistry and related ionic/electronic conduction theories identify that the rate capability of LIBs is kinetically limited by the sluggish solid-state diffusion process in electrode materials. Then, several aspects of the intrinsic materials, materials engineering and processing, and electrode materials architecture design towards maximizing both ionic and electronic conductivity in the electrode with a short diffusion length are deliberated. Finally, the future trends and perspectives for the ultrafast rechargeable LIBs are discussed. Continuous rapid progress in this area is essential and urgent to endow LIBs with ultrafast charging capability to meet huge demands in the near future.

Proton--H/sub 2/ scattering on an ab initio CI potential energy surface. II. Combined vibrational--rotational excitation at 4. 67 and 6 eV

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

Schinke, R.

1980-04-01

Infinite-order-sudden calculations have been performed at 4.67 and 6 eV on the ab initio CI potential energy surface determined recently by Schinke, Dupuis, and Lester. The vibrational degree of freedom has been treated exactly by solving vibrationally coupled radial equations. The rotationally summed differential cross sections for vibrational excitation are in good agreement with the measurements of Schmidt, Hermann, and Linder. It is shown that the rotational excitation cross sections in the vibrational ground state near the rainbow angle are almost exclusively determined by the potential between 2.5a/sub 0/ and 5a/sub 0/ proton--H/sub 2/ separations. In this region only themore » V/sub 2/ term of an expansion into Legendre polynomials is nonvanishing and is a factor of approx.3 smaller for the new surface than for the Giese and Gentry analytic potential. These differences result in a dramatic decrease of the rotational excitation cross sections in the rainbow region so that the present theoretical transition probabilities are in much better agreement with the experiments than our previous sudden vib--rotor calculations utilizing Giese and Gentry's surface.« less

Nonthermal ultrafast optical control of the magnetization in garnet films

NASA Astrophysics Data System (ADS)

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

2006-01-01

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

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.

Photomechanical vibration of thin crystals of polar semiconductors

NASA Technical Reports Server (NTRS)

Lagowski, J.; Gatos, H. C.

1974-01-01

It was found that thin crystals of polar (non-centrosymmetric) semiconductors constitute a new type of photosensitive system in which incident illumination is converted into mechanical energy: thus, illumination-induced elastic deformation (bending) was observed on thin (00.1) CdS and (111) GaAs crystals; furthermore, by employing chopped light the crystals were excited to their resonant vibration (photomechanical vibration); the dependence of the amplitude of this vibration on the energy of the incident radiation was found to be similar to the dependence of the surface photovoltage on the energy of the incident radiation (surface photovoltage spectrum). The present findings are consistent with a model based on light-induced modulation of the piezoelectric surface stresses.

Finite element modelling to assess the effect of surface mounted piezoelectric patch size on vibration response of a hybrid beam

NASA Astrophysics Data System (ADS)

Rahman, N.; Alam, M. N.

2018-02-01

Vibration response analysis of a hybrid beam with surface mounted patch piezoelectric layer is presented in this work. A one dimensional finite element (1D-FE) model based on efficient layerwise (zigzag) theory is used for the analysis. The beam element has eight mechanical and a variable number of electrical degrees of freedom. The beams are also modelled in 2D-FE (ABAQUS) using a plane stress piezoelectric quadrilateral element for piezo layers and a plane stress quadrilateral element for the elastic layers of hybrid beams. Results are presented to assess the effect of size of piezoelectric patch layer on the free and forced vibration responses of thin and moderately thick beams under clamped-free and clamped-clamped configurations. The beams are subjected to unit step loading and harmonic loading to obtain the forced vibration responses. The vibration control using in phase actuation potential on piezoelectric patches is also studied. The 1D-FE results are compared with the 2D-FE results.

Noncontact measurement of vibration using airborne ultrasound.

PubMed

Mater, O B; Remenieras, J P; Bruneel, C; Roncin, A; Patat, F

1998-01-01

A noncontact ultrasonic method for measuring the surface normal vibration of objects was studied. The instrument consists of a pair of 420 kHz ultrasonic air transducers. One is used to emit ultrasounds toward the moving surface, and the other receives the ultrasound reflected from the object under test. Two effects induce a phase modulation on the received signal. The first effect results from the variation of the round trip time interval tau required for the wavefront to go from the emitter to the moving surface and back to the receiver. This is the Doppler effect directly proportional to the surface displacement. The second effect results from the nonlinear parametric interactions of the ultrasonic beams (forward and backward) with the low frequency sound field emitted in the air by the vibrating surface. This latter phenomenon, which is a volume effect, is proportional to the velocity of the vibrating surface and increases with the distance between the transducers and the surface under test. The relative contribution of the Doppler and parametric effects are evaluated, and both have to be taken into account for ultrasonic interferometry in air.

Femtosecond x-ray scattering study of ultrafast photoinduced structural dynamics in solvated [ Co ( terpy ) 2 ] 2 +

DOE PAGES

Biasin, Elisa; van Driel, Tim Brandt; Kjær, Kasper S.; ...

2016-06-30

Here, we study the structural dynamics of photoexcited [Co(terpy) 2] 2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of themore » high spin state is established on a single-picosecond time scale and that this state has a lifetime of ~7 ps.« less

Tracking of the nuclear wavepacket motion in cyanine photoisomerization by ultrafast pump-dump-probe spectroscopy.

PubMed

Wei, Zhengrong; Nakamura, Takumi; Takeuchi, Satoshi; Tahara, Tahei

2011-06-01

Understanding ultrafast reactions, which proceed on a time scale of nuclear motions, requires a quantitative characterization of the structural dynamics. To track such structural changes with time, we studied a nuclear wavepacket motion in photoisomerization of a prototype cyanine dye, 1,1'-diethyl-4,4'-cyanine, by ultrafast pump-dump-probe measurements in solution. The temporal evolution of wavepacket motion was examined by monitoring the efficiency of stimulated emission dumping, which was obtained from the recovery of a ground-state bleaching signal. The dump efficiency versus pump-dump delay exhibited a finite rise time, and it became longer (97 fs → 330 fs → 390 fs) as the dump pulse was tuned to longer wavelengths (690 nm → 950 nm → 1200 nm). This result demonstrates a continuous migration of the leading edge of the wavepacket on the excited-state potential from the Franck-Condon region toward the potential minimum. A slowly decaying feature of the dump efficiency indicated a considerable broadening of the wavepacket over a wide range of the potential, which results in the spread of a population distribution on the flat S(1) potential energy surface. The rapid migration as well as broadening of the wavepacket manifests a continuous nature of the structural dynamics and provides an intuitive visualization of this ultrafast reaction. We also discussed experimental strategies to evaluate reliable dump efficiencies separately from other ultrafast processes and showed a high capability and possibility of the pump-dump-probe method for spectroscopic investigation of unexplored potential regions such as conical intersections. © 2011 American Chemical Society

Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory.

PubMed

Weathersby, S P; Brown, G; Centurion, M; Chase, T F; Coffee, R; Corbett, J; Eichner, J P; Frisch, J C; Fry, A R; Gühr, M; Hartmann, N; Hast, C; Hettel, R; Jobe, R K; Jongewaard, E N; Lewandowski, J R; Li, R K; Lindenberg, A M; Makasyuk, I; May, J E; McCormick, D; Nguyen, M N; Reid, A H; Shen, X; Sokolowski-Tinten, K; Vecchione, T; Vetter, S L; Wu, J; Yang, J; Dürr, H A; Wang, X J

2015-07-01

Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition rate with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability.

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.

Transthoracic Ultrafast Doppler Imaging of Human Left Ventricular Hemodynamic Function

PubMed Central

Osmanski, Bruno-Félix; Maresca, David; Messas, Emmanuel; Tanter, Mickael; Pernot, Mathieu

2016-01-01

Heart diseases can affect intraventricular blood flow patterns. Real-time imaging of blood flow patterns is challenging because it requires both a high frame rate and a large field of view. To date, standard Doppler techniques can only perform blood flow estimation with high temporal resolution within small regions of interest. In this work, we used ultrafast imaging to map in 2D human left ventricular blood flow patterns during the whole cardiac cycle. Cylindrical waves were transmitted at 4800 Hz with a transthoracic phased array probe to achieve ultrafast Doppler imaging of the left ventricle. The high spatio-temporal sampling of ultrafast imaging permits to rely on a much more effective wall filtering and to increase sensitivity when mapping blood flow patterns during the pre-ejection, ejection, early diastole, diastasis and late diastole phases of the heart cycle. The superior sensitivity and temporal resolution of ultrafast Doppler imaging makes it a promising tool for the noninvasive study of intraventricular hemodynamic function. PMID:25073134

Sensor-Based Inspection of the Formation Accuracy in Ultra-Precision Grinding (UPG) of Aspheric Surface Considering the Chatter Vibration

NASA Astrophysics Data System (ADS)

Lei, Yao; Bai, Yue; Xu, Zhijun

2018-06-01

This paper proposes an experimental approach for monitoring and inspection of the formation accuracy in ultra-precision grinding (UPG) with respect to the chatter vibration. Two factors related to the grinding progress, the grinding speed of grinding wheel and spindle, and the oil pressure of the hydrostatic bearing are taken into account to determining the accuracy. In the meantime, a mathematical model of the radius deviation caused by the micro vibration is also established and applied in the experiments. The results show that the accuracy is sensitive to the vibration and the forming accuracy is much improved with proper processing parameters. It is found that the accuracy of aspheric surface can be less than 4 μm when the grinding speed is 1400 r/min and the wheel speed is 100 r/min with the oil pressure being 1.1 MPa.

Transducer senses displacements of panels subjected to vibration

NASA Technical Reports Server (NTRS)

Pea, R. O.

1965-01-01

Inductive vibration sensor measures the surface displacement of nonferrous metal panels subjected to vibration or flutter. This transducer does not make any physical contact with the test panel when measuring.

An advanced molecule-surface scattering instrument for study of vibrational energy transfer in gas-solid collisions.

PubMed

Ran, Qin; Matsiev, Daniel; Wodtke, Alec M; Auerbach, Daniel J

2007-10-01

We describe an advanced and highly sensitive instrument for quantum state-resolved molecule-surface energy transfer studies under ultrahigh vacuum (UHV) conditions. The apparatus includes a beam source chamber, two differential pumping chambers, and a UHV chamber for surface preparation, surface characterization, and molecular beam scattering. Pulsed and collimated supersonic molecular beams are generated by expanding target molecule mixtures through a home-built pulsed nozzle, and excited quantum state-selected molecules were prepared via tunable, narrow-band laser overtone pumping. Detection systems have been designed to measure specific vibrational-rotational state, time-of-flight, angular and velocity distributions of molecular beams coming to and scattered off the surface. Facilities are provided to clean and characterize the surface under UHV conditions. Initial experiments on the scattering of HCl(v = 0) from Au(111) show many advantages of this new instrument for fundamental studies of the energy transfer at the gas-surface interface.

Studies Of Vibrations In Gearboxes

NASA Technical Reports Server (NTRS)

Choy, Fred K.; Ruan, Yeefeng F.; Tu, Yu K.; Zakrajsek, James J.; Oswald, Fred B.; Coy, John J.; Townsend, Dennis P.

1994-01-01

Three NASA technical memorandums summarize studies of vibrations in gearboxes. Directed toward understanding and reducing gearbox noise caused by coupling of vibrations from meshing gears, through gear shafts and their bearings, to surfaces of gearbox housings. Practical systems in which understanding and reduction of gearbox noise beneficial include helicopter, car, and truck transmissions; stationary geared systems; and gear-driven actuator systems.

Vortex Flows in the Liquid Layer and Droplets on a Vibrating Flexible Plate

NASA Astrophysics Data System (ADS)

Aleksandrov, Vladimir; Kopysov, Sergey; Tonkov, Leonid

2018-02-01

In certain conditions, in the layers and droplets of a liquid on a vibrating rectangular flexible plate, vortex flows are formed simultaneously with the excitation of capillary oscillations on the free surface of the liquid layers and droplets. Capillary oscillations in the form of two-dimensional standing waves form Faraday ripples on the free surface of the liquid layer. On the surface of the vibrating droplets, at the excitation of capillary oscillations a light spot reflected from a spotlight source moves along a trajectory in the form of a Lissajous figure observed with a microscope. When vortex flows visualized with graphite microparticles appear in the layer and droplets of a transparent liquid, the trajectory of the light spot on the layer and droplet surface is a two-dimensional trajectory in the form of an ellipse or a saddle. This indicates that the generation of the vortex flows in a liquid at vibrations is due to capillary oscillations in the orthogonally related directions. In the liquid layer and droplets on the surface of the flexible plate, the vibrations of which are generated by bending vibrations, the vortex flows appear due to the plate vibrations and the capillary oscillations of the surface of a layer or a droplet of the liquid. On the free surface of the liquid, the capillary waves, which are parametrically excited by the plate bending vibrations, are additionally modulated by the same bending vibrations in the transverse direction.

Direct diode pumped Ti:sapphire ultrafast regenerative amplifier system

DOE PAGES

Backus, Sterling; Durfee, Charles; Lemons, Randy; ...

2017-02-10

Here, we report on a direct diode-pumped Ti:sapphire ultrafast regenerative amplifier laser system producing multi-uJ energies with repetition rate from 50 to 250 kHz. By combining cryogenic cooling of Ti:sapphire with high brightness fiber-coupled 450nm laser diodes, we for the first time demonstrate a power-scalable CW-pumped architecture that can be directly applied to demanding ultrafast applications such as coherent high-harmonic EUV generation without any complex post-amplification pulse compression. Initial results promise a new era for Ti:sapphire amplifiers not only for ultrafast laser applications, but also for tunable CW sources. We discuss the unique challenges to implementation, as well as themore » solutions to these challenges.« less

Direct diode pumped Ti:sapphire ultrafast regenerative amplifier system

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

Backus, Sterling; Durfee, Charles; Lemons, Randy

Here, we report on a direct diode-pumped Ti:sapphire ultrafast regenerative amplifier laser system producing multi-uJ energies with repetition rate from 50 to 250 kHz. By combining cryogenic cooling of Ti:sapphire with high brightness fiber-coupled 450nm laser diodes, we for the first time demonstrate a power-scalable CW-pumped architecture that can be directly applied to demanding ultrafast applications such as coherent high-harmonic EUV generation without any complex post-amplification pulse compression. Initial results promise a new era for Ti:sapphire amplifiers not only for ultrafast laser applications, but also for tunable CW sources. We discuss the unique challenges to implementation, as well as themore » solutions to these challenges.« less

Earle K. Plyler Prize Lecture: The Three Pillars of Ultrafast Molecular Science - Time, Phase, Intensity

NASA Astrophysics Data System (ADS)

Stolow, Albert

We discuss the probing and control of molecular wavepacket dynamics in the context of three main `pillars' of light-matter interaction: time, phase, intensity. Time: Using short, coherent laser pulses and perturbative matter-field interactions, we study molecular wavepackets with a focus on the ultrafast non-Born-Oppenheimer dynamics, that is, the coupling of electronic and nuclear motions. Time-Resolved Photoelectron Spectroscopy (TRPES) is a powerful ultrafast probe of these processes in polyatomic molecules because it is sensitive both electronic and vibrational dynamics. Ideally, one would like to observe these ultrafast processes from the molecule's point of view - the Molecular Frame - thereby avoiding loss of information due to orientational averaging. This can be achieved by Time-Resolved Coincidence Imaging Spectroscopy (TRCIS) which images 3D recoil vectors of both photofragments and photoelectrons, in coincidence and as a function of time, permitting direct Molecular Frame imaging of valence electronic dynamics during a molecular dynamics. Phase: Using intermediate strength non-perturbative interactions, we apply the second order (polarizability) Non-Resonant Dynamic Stark Effect (NRDSE) to control molecular dynamics without any net absorption of light. NRDSE is also the interaction underlying molecular alignment and applies to field-free 1D of linear molecules and field-free 3D alignment of general (asymmetric) molecules. Using laser alignment, we can transiently fix a molecule in space, yielding a more general approach to direct Molecular Frame imaging of valence electronic dynamics during a chemical reaction. Intensity: In strong (ionizing) laser fields, a new laser-matter physics emerges for polyatomic systems wherein both the single active electron picture and the adiabatic electron response, both implicit in the standard 3-step models, can fail dramatically. This has important consequences for all attosecond strong field spectroscopies of

Intermolecular Vibrations of Hydrophobic Amino Acids

NASA Astrophysics Data System (ADS)

Williams, Michael Roy Casselman

-TDS) was used to measure the absorption spectra of low-frequency vibrational modes for a variety of hydrophobic amino acids in the solid (polycrystalline) state. The THz-TDS technique uses ultrafast (<50 fs) pulses of light from a visible/near-IR laser to generate single-cycle pulses of THz (far-IR) light. Pulses from the ultrafast laser are also used to coherently gate a THz detector, allowing phase-sensitive measurements of the THz electric field. In some cases, Raman scattering spectra of some of the polycrystalline hydrophobic amino acid samples were measured as well, in this case using an Ar+ laser and a triple monochromator to detect signals at the low Raman-shift values corresponding to the far-IR. THz-TDS was used to measure the low-frequency vibrational absorption spectra of pure L- and pure D-valine crystals as well as the racemic cocrystal, DL-valine. As expected, the Land D-valine THz-TDS absorption spectra are identical to one another (they are enantiomorphous crystals) but very different from the spectrum of DL-valine. In the process of these experiments, it was discovered that it was possible to prepare two distinct polymorphs (different crystalline arrangements) of DL-valine by varying the conditions under which stock material was recrystallized. Once crystallized in a particular form, both polymorphs remained (meta)stable at all temperatures investigated (from 80 K to room temperature), i.e., no phase transformation was observed. The THz-TDS and Raman spectra of the two polymorphs of DL-valine were measured. In addition, THz-TDS and Raman spectra of DL-leucine were measured; this substance has a crystal structure closely analagous to one of the DL-valine polymorphs. The temperature-dependence of the THz-TDS spectrum of each material was also measured. At lower temperatures, it is generally expected that intermolecular vibration frequencies increase (blueshift) due to a shrinking unit cell (effectively squeezing the oscillator potential into a smaller space

Experimental study on titanium wire drawing with ultrasonic vibration.

PubMed

Liu, Shen; Shan, Xiaobiao; Guo, Kai; Yang, Yuancai; Xie, Tao

2018-02-01

Titanium and its alloys have been widely used in aerospace and biomedical industries, however, they are classified as difficult-to-machine materials. In this paper, ultrasonic vibration is imposed on the die to overcome the difficulties during conventional titanium wire drawing processes at the room temperature. Numerical simulations were performed to investigate the variation of axial stress within the contacting region and study the change of the drawing stress with several factors in terms of the longitudinal amplitude and frequency of the applied ultrasonic vibration, the diameter reduction ratio, and the drawing force. An experimental testing equipment was established to measure the drawing torque and rotational velocity of the coiler drum during the wire drawing process. The result indicates the drawing force increases with the growth of the drawing velocity and the reduction ratio, whether with or without vibrations. Application of either form of ultrasonic vibrations contributes to the further decrease of the drawing force, especially the longitudinal vibration with larger amplitude. SEM was employed to detect the surface morphology of the processed wires drawn under the three circumstances. The surface quality of the drawn wires with ultrasonic vibrations was apparently improved compared with those using conventional method. In addition, the longitudinal and torsional composite vibration was more effective for surface quality improvement than pure longitudinal vibration, however, at the cost of weakened drawing force reduction effect. Copyright © 2017 Elsevier B.V. All rights reserved.

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

Fingertip contact suppresses the destabilizing influence of leg muscle vibration

NASA Technical Reports Server (NTRS)

Lackner, J. R.; Rabin, E.; DiZio, P.

2000-01-01

Touch of the hand with a stationary surface at nonmechanically supportive force levels (<1 N) greatly attenuates postural sway during quiet stance. We predicted such haptic contact would also suppress the postural destabilization caused by vibrating the right peroneus brevis and longus muscles of subjects standing heel-to-toe with eyes closed. In experiment 1, ten subjects were tested under four conditions: no-vibration, no-touch; no-vibration, touch; vibration, no-touch; and vibration, touch. A hand-held physiotherapy vibrator (120 Hz) was applied approximately 5 cm above the malleolous to stimulate the peroneus longus and brevis tendons. Touch conditions involved contact of the right index finger with a laterally positioned surface (<1 N of force) at waist height. Vibration in the absence of finger contact greatly increased the mean sway amplitude of the center of pressure and of the head relative to the no-vibration, no-touch control condition (P < 0.001). The touch, no-vibration and touch-vibration conditions were not significantly different (P > 0.05) from each other and both had significantly less mean sway amplitude of head and of center of pressure than the other conditions (P < 0.01). In experiment 2, eight subjects stood heel-to-toe under touch and no-touch conditions involving 40-s duration trials of peroneus tendon vibration at different duty cycles: 1-, 2-, 3-, and 4-s ON and OFF periods. The vibrator was attached to the subject's leg and remotely activated. In the no-touch conditions, subjects showed periodic postural disruptions contingent on the duty cycle and mirror image rebounds with the offset of vibration. In the touch conditions, subjects were much less disrupted and showed compensations occurring within 500 ms of vibration onset and mirror image rebounds with vibration offset. Subjects were able to suppress almost completely the destabilizing influence of the vibration in the 3- and 4-s duty cycle trials. These experiments show that haptic

An ultrafast X-ray scintillating detector made of ZnO(Ga)

NASA Astrophysics Data System (ADS)

Zhang, Qingmin; Yan, Jun; Deng, Bangjie; Zhang, Jingwen; Lv, Jinge; Wen, Xin; Gao, Keqing

2017-12-01

Owing to its ultrafast scintillation, quite high light yield, strong radiation resistance, and non-deliquescence, ZnO(Ga) is a highly promising choice for an ultrafast X-ray detector. Because of its high deposition rate, good production repeatability and strong adhesive force, reactive magnetron sputtering was used to produce a ZnO(Ga) crystal on a quartz glass substrate, after the production conditions were optimized. The fluorescence lifetime of the sample was 173 ps. An ultrafast X-ray scintillating detector, equipped with a fast microchannel plate (MCP) photomultiplier tube (PMT), was developed and the X-ray tests show a signal full width at half maximum (FWHM) of only 385.5 ps. Moreover, derivation from the previous measurement shows the ZnO(Ga) has an ultrafast time response (FWHM = 355.1 ps) and a high light yield (14740 photons/MeV).

Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory

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

Weathersby, S. P.; Brown, G.; Chase, T. F.

Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition ratemore » with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability.« less

Vibration on board and health effects.

PubMed

Jensen, Anker; Jepsen, Jørgen Riis

2014-01-01

There is only limited knowledge of the exposure to vibrations of ships' crews and their risk of vibration-induced health effects. Exposure to hand-arm vibrations from the use of vibrating tools at sea does not differ from that in the land-based trades. However, in contrast to most other work places, seafarers are also exposed to vibrations to the feet when standing on vibrating surfaces on board. Anecdotal reports have related the development of "white feet" to local exposure to vibration, e.g. in mining, but this connection has not been investigated in the maritime setting. As known from studies of the health consequences of whole body vibrations in land-transportation, such exposure at sea may affect ships' passengers and crews. While the relation of back disorders to high levels of whole body vibration has been demonstrated among e.g. tractor drivers, there are no reported epidemiological evidence for such relation among seafarers except for fishermen, who, however, are also exposed to additional recognised physical risk factors at work. The assessment and reduction of vibrations by naval architects relates to technical implications of this impact for the ships' construction, but has limited value for the estimation of health risks because they express the vibration intensity differently that it is done in a medical context.

Engineering model for ultrafast laser microprocessing

NASA Astrophysics Data System (ADS)

Audouard, E.; Mottay, E.

2016-03-01

Ultrafast laser micro-machining relies on complex laser-matter interaction processes, leading to a virtually athermal laser ablation. The development of industrial ultrafast laser applications benefits from a better understanding of these processes. To this end, a number of sophisticated scientific models have been developed, providing valuable insights in the physics of the interaction. Yet, from an engineering point of view, they are often difficult to use, and require a number of adjustable parameters. We present a simple engineering model for ultrafast laser processing, applied in various real life applications: percussion drilling, line engraving, and non normal incidence trepanning. The model requires only two global parameters. Analytical results are derived for single pulse percussion drilling or simple pass engraving. Simple assumptions allow to predict the effect of non normal incident beams to obtain key parameters for trepanning drilling. The model is compared to experimental data on stainless steel with a wide range of laser characteristics (time duration, repetition rate, pulse energy) and machining conditions (sample or beam speed). Ablation depth and volume ablation rate are modeled for pulse durations from 100 fs to 1 ps. Trepanning time of 5.4 s with a conicity of 0.15° is obtained for a hole of 900 μm depth and 100 μm diameter.

Femtosecond characterization of vibrational optical activity of chiral molecules.

PubMed

Rhee, Hanju; June, Young-Gun; Lee, Jang-Soo; Lee, Kyung-Koo; Ha, Jeong-Hyon; Kim, Zee Hwan; Jeon, Seung-Joon; Cho, Minhaeng

2009-03-19

Optical activity is the result of chiral molecules interacting differently with left versus right circularly polarized light. Because of this intrinsic link to molecular structure, the determination of optical activity through circular dichroism (CD) spectroscopy has long served as a routine method for obtaining structural information about chemical and biological systems in condensed phases. A recent development is time-resolved CD spectroscopy, which can in principle map the structural changes associated with biomolecular function and thus lead to mechanistic insights into fundamental biological processes. But implementing time-resolved CD measurements is experimentally challenging because CD is a notoriously weak effect (a factor of 10(-4)-10(-6) smaller than absorption). In fact, this problem has so far prevented time-resolved vibrational CD experiments. Here we show that vibrational CD spectroscopy with femtosecond time resolution can be realized when using heterodyned spectral interferometry to detect the phase and amplitude of the infrared optical activity free-induction-decay field in time (much like in a pulsed NMR experiment). We show that we can detect extremely weak signals in the presence of large achiral background contributions, by simultaneously measuring with a femtosecond laser pulse the vibrational CD and optical rotatory dispersion spectra of dissolved chiral limonene molecules. We have so far only targeted molecules in equilibrium, but it would be straightforward to extend the method for the observation of ultrafast structural changes such as those occurring during protein folding or asymmetric chemical reactions. That is, we should now be in a position to produce 'molecular motion pictures' of fundamental molecular processes from a chiral perspective.

Experimental realization of quantum teleportation from a photon to the vibration modes of a millimeter-sized diamond

NASA Astrophysics Data System (ADS)

Huang, Yuanyuan; Hou, Panyu; Yuan, Xinxing; Chang, Xiuying; Zu, Chong; He, Li; Duan, Luming; CenterQuantum Information, IIIS, Tsinghua University, Beijing 100084, PR China Team; Department of Physics, University of Michigan, Ann Arbor, Michigan 48109, USA Team

2016-05-01

Quantum teleportation is of great importance to various quantum technologies, and has been realized between light beams, trapped atoms, superconducting qubits, and defect spins in solids. Here we report an experimental demonstration of quantum teleportation from light beams to vibrational states of a macroscopic diamond under ambient conditions. In our experiment, the ultrafast laser technology provides the key tool for fast processing and detection of quantum states within its short life time in macroscopic objects consisting of many strongly interacting atoms that are coupled to the environment, and finally we demonstrate an average teleportation fidelity (90 . 6 +/- 1 . 0) % , clearly exceeding the classical limit of 2/3. Quantum control of the optomechanical coupling may provide efficient ways for realization of transduction of quantum signals, processing of quantum information, and sensing of small mechanical vibrations. Center for Quantum Information, IIIS, Tsinghua University, Beijing 100084, PR China.

Moving contact lines on vibrating surfaces

NASA Astrophysics Data System (ADS)

Solomenko, Zlatko; Spelt, Peter; Scott, Julian

2017-11-01

Large-scale simulations of flows with moving contact lines for realistic conditions generally requires a subgrid scale model (analyses based on matched asymptotics) to account for the unresolved part of the flow, given the large range of length scales involved near contact lines. Existing models for the interface shape in the contact-line region are primarily for steady flows on homogeneous substrates, with encouraging results in 3D simulations. Introduction of complexities would require further investigation of the contact-line region, however. Here we study flows with moving contact lines on planar substrates subject to vibrations, with applications in controlling wetting/dewetting. The challenge here is to determine the change in interface shape near contact lines due to vibrations. To develop further insight, 2D direct numerical simulations (wherein the flow is resolved down to an imposed slip length) have been performed to enable comparison with asymptotic theory, which is also developed further. Perspectives will also be presented on the final objective of the work, which is to develop a subgrid scale model that can be utilized in large-scale simulations. The authors gratefully acknowledge the ANR for financial support (ANR-15-CE08-0031) and the meso-centre FLMSN for use of computational resources. This work was Granted access to the HPC resources of CINES under the allocation A0012B06893 made by GENCI.

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

Carrier dynamics and surface vibration-assisted Auger recombination in porous silicon

NASA Astrophysics Data System (ADS)

Zakar, Ammar; Wu, Rihan; Chekulaev, Dimitri; Zerova, Vera; He, Wei; Canham, Leigh; Kaplan, Andrey

2018-04-01

Excitation and recombination dynamics of the photoexcited charge carriers in porous silicon membranes were studied using a femtosecond pump-probe technique. Near-infrared pulses (800 nm, 60 fs) were used for the pump while, for the probe, we employed different wavelengths in the range between 3.4 and 5 μ m covering the medium wavelength infrared range. The data acquired in these experiments consist of simultaneous measurements of the transmittance and reflectance as a function of the delay time between the pump and probe for different pump fluences and probe wavelengths. To evaluate the results, we developed an optical model based on the two-dimensional Maxwell-Garnett formula, incorporating the free-carrier Drude contribution and nonuniformity of the excitation by the Wentzel-Kramers-Brillouin model. This model allowed the retrieval of information about the carrier density as a function of the pump fluence, time, and wavelength. The carrier density data were analyzed to reveal that the recombination dynamics is governed by Shockley-Read-Hall and Auger processes, whereas the diffusion has an insignificant contribution. We show that, in porous silicon samples, the Auger recombination process is greatly enhanced at the wavelength corresponding to the infrared-active vibrational modes of the molecular impurities on the surface of the pores. This observation of surface-vibration-assisted Auger recombination is not only for porous silicon in particular, but for low-dimension and bulk semiconductors in general. We estimate the time constants of Shockley-Read-Hall and Auger processes, and demonstrate their wavelength dependence for the excited carrier density in the range of 1018-10191 /cm3 . We demonstrate that both processes are enhanced by up to three orders of magnitude with respect to the bulk counterpart. In addition, we provide a plethora of the physical parameters evaluated from the experimental data, such as the dielectric function and its dependence on the

Dynamic surface acoustic response to a thermal expansion source on an anisotropic half space.

PubMed

Zhao, Peng; Zhao, Ji-Cheng; Weaver, Richard

2013-05-01

The surface displacement response to a distributed thermal expansion source is solved using the reciprocity principle. By convolving the strain Green's function with the thermal stress field created by an ultrafast laser illumination, the complete surface displacement on an anisotropic half space induced by laser absorption is calculated in the time domain. This solution applies to the near field surface displacement due to pulse laser absorption. The solution is validated by performing ultrafast laser pump-probe measurements and showing very good agreement between the measured time-dependent probe beam deflection and the computed surface displacement.

Ultrafast shock compression of self-assembled monolayers: a molecular picture.

PubMed

Patterson, James E; Dlott, Dana D

2005-03-24

Simulations of self-assembled monolayers (SAMs) are performed to interpret experimental measurements of ultrafast approximately 1 GPa (volume compression deltaV approximately 0.1) planar shock compression dynamics probed by vibrational sum-frequency generation (SFG) spectroscopy (Lagutchev, A. S.; Patterson, J. E.; Huang, W.; Dlott, D. D. J. Phys. Chem. B 2005, 109, XXXX). The SAMs investigated are octadecanethiol (ODT) and pentadecanethiol (PDT) on Au(111) and Ag(111) substrates, and benzyl mercaptan (BMT) on Au(111). In the alkane SAMs, SFG is sensitive to the instantaneous orientation of the terminal methyl; in BMT it is sensitive to the phenyl orientation. Computed structures of alkane SAMs are in good agreement with experiment. In alkanes, the energies of gauche defects increase with increasing number and depth below the methyl plane, with the exception of ODT/Au where both single and double gauche defects at the two uppermost dihedrals have similar energies. Simulations of isothermal uniaxial compression of SAM lattices show that chain and methyl tilting is predominant in PDT/Au, ODT/Ag and PDT/Ag, whereas single and double gauche defect formation is predominant in ODT/Au. Time-resolved shock data showing transient SFG signal loss of ODT/Au and PDT/Au are fit by calculations of the terminal group orientations as a function of deltaV and their contributions to the SFG hyperpolarizability. The highly elastic response of PDT/Au results from shock-generated methyl and chain tilting. The viscoelastic response of ODT/Au results from shock generation of single and double gauche defects. Isothermal compression simulations help explain and fit the time dependence of shock spectra but generally underestimate the magnitude of SFG signal loss because they do not include effects of high-strain-rate dynamics and shock front and surface irregularities.

Ultrafast lattice dynamics of single crystal and polycrystalline gold nanofilms☆

NASA Astrophysics Data System (ADS)

Hu, Jianbo; Karam, Tony E.; Blake, Geoffrey A.; Zewail, Ahmed H.

2017-09-01

Ultrafast electron diffraction is employed to spatiotemporally visualize the lattice dynamics of 11 nm-thick single-crystal and 2 nm-thick polycrystalline gold nanofilms. Surprisingly, the electron-phonon coupling rates derived from two temperature simulations of the data reveal a faster interaction between electrons and the lattice in the case of the single-crystal sample. We interpret this unexpected behavior as arising from quantum confinement of the electrons in the 2 nm-thick gold nanofilm, as supported by absorption spectra, an effect that counteracts the expected increase in the electron scattering off surfaces and grain boundaries in the polycrystalline materials.

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 Growth of High-Quality Monolayer WSe2 on Au.

PubMed

Gao, Yang; Hong, Yi-Lun; Yin, Li-Chang; Wu, Zhangting; Yang, Zhiqing; Chen, Mao-Lin; Liu, Zhibo; Ma, Teng; Sun, Dong-Ming; Ni, Zhenhua; Ma, Xiu-Liang; Cheng, Hui-Ming; Ren, Wencai

2017-08-01

The ultrafast growth of high-quality uniform monolayer WSe 2 is reported with a growth rate of ≈26 µm s -1 by chemical vapor deposition on reusable Au substrate, which is ≈2-3 orders of magnitude faster than those of most 2D transition metal dichalcogenides grown on nonmetal substrates. Such ultrafast growth allows for the fabrication of millimeter-size single-crystal WSe 2 domains in ≈30 s and large-area continuous films in ≈60 s. Importantly, the ultrafast grown WSe 2 shows excellent crystal quality and extraordinary electrical performance comparable to those of the mechanically exfoliated samples, with a high mobility up to ≈143 cm 2 V -1 s -1 and ON/OFF ratio up to 9 × 10 6 at room temperature. Density functional theory calculations reveal that the ultrafast growth of WSe 2 is due to the small energy barriers and exothermic characteristic for the diffusion and attachment of W and Se on the edges of WSe 2 on Au substrate. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Amplification of an Autodyne Signal in a Bistable Vertical-Cavity Surface-Emitting Laser with the Use of a Vibrational Resonance

NASA Astrophysics Data System (ADS)

Chizhevsky, V. N.

2018-01-01

For the first time, it is demonstrated experimentally that a vibrational resonance in a polarization-bistable vertical-cavity surface-emitting laser can be used to increase the laser response in autodyne detection of microvibrations from reflecting surfaces. In this case, more than 25-fold signal amplification is achieved. The influence of the asymmetry of the bistable potential on the microvibration-detection efficiency is studied.

Calculation of acoustic field based on laser-measured vibration velocities on ultrasonic transducer surface

NASA Astrophysics Data System (ADS)

Hu, Liang; Zhao, Nannan; Gao, Zhijian; Mao, Kai; Chen, Wenyu; Fu, Xin

2018-05-01

Determination of the distribution of a generated acoustic field is valuable for studying ultrasonic transducers, including providing the guidance for transducer design and the basis for analyzing their performance, etc. A method calculating the acoustic field based on laser-measured vibration velocities on the ultrasonic transducer surface is proposed in this paper. Without knowing the inner structure of the transducer, the acoustic field outside it can be calculated by solving the governing partial differential equation (PDE) of the field based on the specified boundary conditions (BCs). In our study, the BC on the transducer surface, i.e. the distribution of the vibration velocity on the surface, is accurately determined by laser scanning measurement of discrete points and follows a data fitting computation. In addition, to ensure the calculation accuracy for the whole field even in an inhomogeneous medium, a finite element method is used to solve the governing PDE based on the mixed BCs, including the discretely measured velocity data and other specified BCs. The method is firstly validated on numerical piezoelectric transducer models. The acoustic pressure distributions generated by a transducer operating in an homogeneous and inhomogeneous medium, respectively, are both calculated by the proposed method and compared with the results from other existing methods. Then, the method is further experimentally validated with two actual ultrasonic transducers used for flow measurement in our lab. The amplitude change of the output voltage signal from the receiver transducer due to changing the relative position of the two transducers is calculated by the proposed method and compared with the experimental data. This method can also provide the basis for complex multi-physical coupling computations where the effect of the acoustic field should be taken into account.

Ultrafast magnetodynamics with free-electron lasers

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

Response to Tendon Vibration Questions the Underlying Rationale of Proprioceptive Training

PubMed Central

Lubetzky, Anat Vilnai; McCoy, Sarah Westcott; Price, Robert; Kartin, Deborah

2017-01-01

Context: Proprioceptive training on compliant surfaces is used to rehabilitate and prevent ankle sprains. The ability to improve proprioceptive function via such training has been questioned. Achilles tendon vibration is used in motor-control research as a form of proprioceptive stimulus. Using measures of postural steadiness with nonlinear measures to elucidate control mechanisms, tendon vibration can be applied to investigate the underlying rationale of proprioceptive training. Objective: To test whether the effect of vibration on young adults' postural control depended on the support surface. Design: Descriptive laboratory study. Setting: Research laboratory. Patients or Other Participants: Thirty healthy adults and 10 adults with chronic ankle instability (CAI; age range = 18−40 years). Intervention(s): With eyes open, participants stood in bilateral stance on a rigid plate (floor), memory foam, and a Both Sides Up (BOSU) ball covering a force platform. We applied bilateral Achilles tendon vibration for the middle 20 seconds in a series of 60-second trials and analyzed participants' responses from previbration to vibration (pre-vib) and from vibration to postvibration (vib-post). Main Outcome Measure(s): We calculated anterior-posterior excursion of the center of pressure and complexity index derived from the area under multiscale entropy curves. Results: The excursion response to vibration differed by surface, as indicated by a significant interaction of P < .001 for the healthy group at both time points and for the CAI group vib-post. Although both groups demonstrated increased excursion from pre-vib and from vib-post, a decrease was observed on the BOSU. The complexity response to vibration differed by surface for the healthy group (pre-vib, P < .001). The pattern for the CAI group was similar but not significant. Complexity changes vib-post were the same on all surfaces for both groups. Conclusions: Participants reacted less to ankle vibration when

Response to Tendon Vibration Questions the Underlying Rationale of Proprioceptive Training.

PubMed

Lubetzky, Anat Vilnai; McCoy, Sarah Westcott; Price, Robert; Kartin, Deborah

2017-02-01

Proprioceptive training on compliant surfaces is used to rehabilitate and prevent ankle sprains. The ability to improve proprioceptive function via such training has been questioned. Achilles tendon vibration is used in motor-control research as a form of proprioceptive stimulus. Using measures of postural steadiness with nonlinear measures to elucidate control mechanisms, tendon vibration can be applied to investigate the underlying rationale of proprioceptive training. To test whether the effect of vibration on young adults' postural control depended on the support surface. Descriptive laboratory study. Research laboratory. Thirty healthy adults and 10 adults with chronic ankle instability (CAI; age range = 18-40 years). With eyes open, participants stood in bilateral stance on a rigid plate (floor), memory foam, and a Both Sides Up (BOSU) ball covering a force platform. We applied bilateral Achilles tendon vibration for the middle 20 seconds in a series of 60-second trials and analyzed participants' responses from previbration to vibration (pre-vib) and from vibration to postvibration (vib-post). We calculated anterior-posterior excursion of the center of pressure and complexity index derived from the area under multiscale entropy curves. The excursion response to vibration differed by surface, as indicated by a significant interaction of P < .001 for the healthy group at both time points and for the CAI group vib-post. Although both groups demonstrated increased excursion from pre-vib and from vib-post, a decrease was observed on the BOSU. The complexity response to vibration differed by surface for the healthy group (pre-vib, P < .001). The pattern for the CAI group was similar but not significant. Complexity changes vib-post were the same on all surfaces for both groups. Participants reacted less to ankle vibration when standing on the BOSU as compared with the floor, suggesting that proprioceptive training may not be occurring. Different balance

Ultrafast surface modification of Ni3S2 nanosheet arrays with Ni-Mn bimetallic hydroxides for high-performance supercapacitors.

PubMed

Zou, Xu; Sun, Qing; Zhang, Yuxin; Li, Guo-Dong; Liu, Yipu; Wu, Yuanyuan; Yang, Lan; Zou, Xiaoxin

2018-03-14

Amorphous Ni-Mn bimetallic hydroxide film on the three-dimensional nickle foam (NF)-supported conductive Ni 3 S 2 nanosheets (denoted as Ni-Mn-OH@Ni 3 S 2 /NF) is successfully synthesized by an ultrafast process (5 s). The fascinating structural characteristic endows Ni-Mn-OH@Ni 3 S 2 /NF electrodes better electrochemical performance. The specific capacitance of 2233.3 F g -1 at a current density of 15 A g -1 can achieve high current density charge and discharge at 20/30 A g -1 that the corresponding capacitance is 1529.16 and 1350 F g -1 , respectively. As well as good cycling performance after 1000 cycles can maintain 72% at 15 A g -1 . The excellent performance can be attributed to unique surface modification nanostructures and the synergistic effect of the bimetallic hydroxide film. The impressive results provide new opportunity to produce advanced electrode materials by simple and green route and this material is expected to apply in high energy density storage systems.

Indirect excitation of ultrafast demagnetization

DOE PAGES

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

2016-01-06

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

Indirect excitation of ultrafast demagnetization

PubMed Central