Ultrafast transmission electron microscopy using a laser-driven field emitter: Femtosecond resolution with a high coherence electron beam.

PubMed

Feist, Armin; Bach, Nora; Rubiano da Silva, Nara; Danz, Thomas; Möller, Marcel; Priebe, Katharina E; Domröse, Till; Gatzmann, J Gregor; Rost, Stefan; Schauss, Jakob; Strauch, Stefanie; Bormann, Reiner; Sivis, Murat; Schäfer, Sascha; Ropers, Claus

2017-05-01

We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the Göttingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in ultrafast electron microscopy of 9Å focused beam diameter, 200fs pulse duration and 0.6eV energy width. We illustrate the possibility to conduct ultrafast imaging, diffraction, holography and spectroscopy with this instrument and also discuss opportunities to harness quantum coherent interactions between intense laser fields and free-electron beams. Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.

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

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

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

2015-12-28

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

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.

Ultrafast Harmonic Coherent Compound (UHCC) imaging for high frame rate echocardiography and Shear Wave Elastography

PubMed Central

Correia, Mafalda; Provost, Jean; Chatelin, Simon; Villemain, Olivier; Tanter, Mickael; Pernot, Mathieu

2016-01-01

Transthoracic shear wave elastography of the myocardium remains very challenging due to the poor quality of transthoracic ultrafast imaging and the presence of clutter noise, jitter, phase aberration, and ultrasound reverberation. Several approaches, such as, e.g., diverging-wave coherent compounding or focused harmonic imaging have been proposed to improve the imaging quality. In this study, we introduce ultrafast harmonic coherent compounding (UHCC), in which pulse-inverted diverging-waves are emitted and coherently compounded, and show that such an approach can be used to enhance both Shear Wave Elastography (SWE) and high frame rate B-mode Imaging. UHCC SWE was first tested in phantoms containing an aberrating layer and was compared against pulse-inversion harmonic imaging and against ultrafast coherent compounding (UCC) imaging at the fundamental frequency. In-vivo feasibility of the technique was then evaluated in six healthy volunteers by measuring myocardial stiffness during diastole in transthoracic imaging. We also demonstrated that improvements in imaging quality could be achieved using UHCC B-mode imaging in healthy volunteers. The quality of transthoracic images of the heart was found to be improved with the number of pulse-inverted diverging waves with reduction of the imaging mean clutter level up to 13.8-dB when compared against UCC at the fundamental frequency. These results demonstrated that UHCC B-mode imaging is promising for imaging deep tissues exposed to aberration sources with a high frame-rate. PMID:26890730

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

DOE PAGES

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

2015-10-28

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

Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics

NASA Astrophysics Data System (ADS)

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

2016-08-01

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

Complete coherent control of silicon vacancies in diamond nanopillars containing single defect centers

DOE PAGES

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan -Kai; ...

2017-10-23

Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon-vacancy (SiV) centers in diamond offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye–Waller factor. The possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times makes them promising candidates for qubits. Here, we have developed arrays of nanopillars containing single (SiV) centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the excited state population of a single SiV center at the opticalmore » transition frequency. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the excited state population of individual SiV centers on picosecond timescales using ultrafast optical pulses. Furthermore, this work opens new opportunities to create a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.« less

Complete coherent control of silicon vacancies in diamond nanopillars containing single defect centers

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

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan -Kai

Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon-vacancy (SiV) centers in diamond offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye–Waller factor. The possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times makes them promising candidates for qubits. Here, we have developed arrays of nanopillars containing single (SiV) centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the excited state population of a single SiV center at the opticalmore » transition frequency. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the excited state population of individual SiV centers on picosecond timescales using ultrafast optical pulses. Furthermore, this work opens new opportunities to create a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.« less

Real-time and sub-wavelength ultrafast coherent diffraction imaging in the extreme ultraviolet.

PubMed

Zürch, M; Rothhardt, J; Hädrich, S; Demmler, S; Krebs, M; Limpert, J; Tünnermann, A; Guggenmos, A; Kleineberg, U; Spielmann, C

2014-12-08

Coherent Diffraction Imaging is a technique to study matter with nanometer-scale spatial resolution based on coherent illumination of the sample with hard X-ray, soft X-ray or extreme ultraviolet light delivered from synchrotrons or more recently X-ray Free-Electron Lasers. This robust technique simultaneously allows quantitative amplitude and phase contrast imaging. Laser-driven high harmonic generation XUV-sources allow table-top realizations. However, the low conversion efficiency of lab-based sources imposes either a large scale laser system or long exposure times, preventing many applications. Here we present a lensless imaging experiment combining a high numerical aperture (NA = 0.8) setup with a high average power fibre laser driven high harmonic source. The high flux and narrow-band harmonic line at 33.2 nm enables either sub-wavelength spatial resolution close to the Abbe limit (Δr = 0.8λ) for long exposure time, or sub-70 nm imaging in less than one second. The unprecedented high spatial resolution, compactness of the setup together with the real-time capability paves the way for a plethora of applications in fundamental and life sciences.

Optical laser systems at the Linac Coherent Light Source

DOE PAGES

Minitti, Michael P.; Robinson, Joseph S.; Coffee, Ryan N.; ...

2015-04-22

Ultrafast optical lasers play an essential role in exploiting the unique capabilities of recently commissioned X-ray free-electron laser facilities such as the Linac Coherent Light Source (LCLS). Pump–probe experimental techniques reveal ultrafast dynamics in atomic and molecular processes and reveal new insights in chemistry, biology, material science and high-energy-density physics. This manuscript describes the laser systems and experimental methods that enable cutting-edge optical laser/X-ray pump–probe experiments to be performed at LCLS.

Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics

PubMed Central

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

2016-01-01

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

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

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

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.

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

NASA Astrophysics Data System (ADS)

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

2017-06-01

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

Quantum coherent optical phase modulation in an ultrafast transmission electron microscope.

PubMed

Feist, Armin; Echternkamp, Katharina E; Schauss, Jakob; Yalunin, Sergey V; Schäfer, Sascha; Ropers, Claus

2015-05-14

Coherent manipulation of quantum systems with light is expected to be a cornerstone of future information and communication technology, including quantum computation and cryptography. The transfer of an optical phase onto a quantum wavefunction is a defining aspect of coherent interactions and forms the basis of quantum state preparation, synchronization and metrology. Light-phase-modulated electron states near atoms and molecules are essential for the techniques of attosecond science, including the generation of extreme-ultraviolet pulses and orbital tomography. In contrast, the quantum-coherent phase-modulation of energetic free-electron beams has not been demonstrated, although it promises direct access to ultrafast imaging and spectroscopy with tailored electron pulses on the attosecond scale. Here we demonstrate the coherent quantum state manipulation of free-electron populations in an electron microscope beam. We employ the interaction of ultrashort electron pulses with optical near-fields to induce Rabi oscillations in the populations of electron momentum states, observed as a function of the optical driving field. Excellent agreement with the scaling of an equal-Rabi multilevel quantum ladder is obtained, representing the observation of a light-driven 'quantum walk' coherently reshaping electron density in momentum space. We note that, after the interaction, the optically generated superposition of momentum states evolves into a train of attosecond electron pulses. Our results reveal the potential of quantum control for the precision structuring of electron densities, with possible applications ranging from ultrafast electron spectroscopy and microscopy to accelerator science and free-electron lasers.

Quantum coherent optical phase modulation in an ultrafast transmission electron microscope

NASA Astrophysics Data System (ADS)

Feist, Armin; Echternkamp, Katharina E.; Schauss, Jakob; Yalunin, Sergey V.; Schäfer, Sascha; Ropers, Claus

2015-05-01

Coherent manipulation of quantum systems with light is expected to be a cornerstone of future information and communication technology, including quantum computation and cryptography. The transfer of an optical phase onto a quantum wavefunction is a defining aspect of coherent interactions and forms the basis of quantum state preparation, synchronization and metrology. Light-phase-modulated electron states near atoms and molecules are essential for the techniques of attosecond science, including the generation of extreme-ultraviolet pulses and orbital tomography. In contrast, the quantum-coherent phase-modulation of energetic free-electron beams has not been demonstrated, although it promises direct access to ultrafast imaging and spectroscopy with tailored electron pulses on the attosecond scale. Here we demonstrate the coherent quantum state manipulation of free-electron populations in an electron microscope beam. We employ the interaction of ultrashort electron pulses with optical near-fields to induce Rabi oscillations in the populations of electron momentum states, observed as a function of the optical driving field. Excellent agreement with the scaling of an equal-Rabi multilevel quantum ladder is obtained, representing the observation of a light-driven `quantum walk' coherently reshaping electron density in momentum space. We note that, after the interaction, the optically generated superposition of momentum states evolves into a train of attosecond electron pulses. Our results reveal the potential of quantum control for the precision structuring of electron densities, with possible applications ranging from ultrafast electron spectroscopy and microscopy to accelerator science and free-electron lasers.

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

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

Sartorello, Giovanni; Olivier, Nicolas; Zhang, Jingjing

2016-08-17

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

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

Transient ultrafast coherent spectroscopy of 2-propanol

NASA Astrophysics Data System (ADS)

Meiselman, Seth; Decamp, Matthew; Lorenz, Virginia

We use transient coherent spontaneous Raman spectroscopy to measure the coherence lifetimes of vibrational states in liquid propanol. By creating single-photon-level collective excitations of the vibrational states in the system we observe coherence oscillations due to simultaneous excitation of the 2885 cm-1, 2938 cm-1, and 2976 cm-1 modes. These lifetimes and oscillation frequencies agree with frequency-domain lineshape measurements.

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

PubMed

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

2012-07-05

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

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

NASA Astrophysics Data System (ADS)

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

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

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

NASA Astrophysics Data System (ADS)

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

2016-09-01

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

3-D ultrafast Doppler imaging applied to the noninvasive mapping of blood vessels in vivo.

PubMed

Provost, Jean; Papadacci, Clement; Demene, Charlie; Gennisson, Jean-Luc; Tanter, Mickael; Pernot, Mathieu

2015-08-01

Ultrafast Doppler imaging was introduced as a technique to quantify blood flow in an entire 2-D field of view, expanding the field of application of ultrasound imaging to the highly sensitive anatomical and functional mapping of blood vessels. We have recently developed 3-D ultrafast ultrasound imaging, a technique that can produce thousands of ultrasound volumes per second, based on a 3-D plane and diverging wave emissions, and demonstrated its clinical feasibility in human subjects in vivo. In this study, we show that noninvasive 3-D ultrafast power Doppler, pulsed Doppler, and color Doppler imaging can be used to perform imaging of blood vessels in humans when using coherent compounding of 3-D tilted plane waves. A customized, programmable, 1024-channel ultrasound system was designed to perform 3-D ultrafast imaging. Using a 32 × 32, 3-MHz matrix phased array (Vermon, Tours, France), volumes were beamformed by coherently compounding successive tilted plane wave emissions. Doppler processing was then applied in a voxel-wise fashion. The proof of principle of 3-D ultrafast power Doppler imaging was first performed by imaging Tygon tubes of various diameters, and in vivo feasibility was demonstrated by imaging small vessels in the human thyroid. Simultaneous 3-D color and pulsed Doppler imaging using compounded emissions were also applied in the carotid artery and the jugular vein in one healthy volunteer.

3-D Ultrafast Doppler Imaging Applied to the Noninvasive and Quantitative Imaging of Blood Vessels in Vivo

PubMed Central

Provost, J.; Papadacci, C.; Demene, C.; Gennisson, J-L.; Tanter, M.; Pernot, M.

2016-01-01

Ultrafast Doppler Imaging was introduced as a technique to quantify blood flow in an entire 2-D field of view, expanding the field of application of ultrasound imaging to the highly sensitive anatomical and functional mapping of blood vessels. We have recently developed 3-D Ultrafast Ultrasound Imaging, a technique that can produce thousands of ultrasound volumes per second, based on three-dimensional plane and diverging wave emissions, and demonstrated its clinical feasibility in human subjects in vivo. In this study, we show that non-invasive 3-D Ultrafast Power Doppler, Pulsed Doppler, and Color Doppler Imaging can be used to perform quantitative imaging of blood vessels in humans when using coherent compounding of three-dimensional tilted plane waves. A customized, programmable, 1024-channel ultrasound system was designed to perform 3-D Ultrafast Imaging. Using a 32X32, 3-MHz matrix phased array (Vermon, France), volumes were beamformed by coherently compounding successive tilted plane wave emissions. Doppler processing was then applied in a voxel-wise fashion. 3-D Ultrafast Power Doppler Imaging was first validated by imaging Tygon tubes of varying diameter and its in vivo feasibility was demonstrated by imaging small vessels in the human thyroid. Simultaneous 3-D Color and Pulsed Doppler Imaging using compounded emissions were also applied in the carotid artery and the jugular vein in one healthy volunteer. PMID:26276956

Ultrafast Saturation of Electronic-Resonance-Enhanced Coherent Anti-Stokes Raman Scattering and Comparison for Pulse Durations in the Nanosecond to Femtosecond Regime

DTIC Science & Technology

2016-02-05

electronic-resonance-enhanced CARS (ERE- CARS ) configuration is calculated. We demonstrate that while underdamping condition is a suffi- cient condition for...saturation of ERE- CARS with the long-pulse excitations, a transient-gain must be achieved to saturate ERE- CARS signal for ultrafast probe regime. We...ultrafast ERE- CARS . From a simplified analytical solution and a detailed numerical calculation based on density-matrix equations, the saturation threshold

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.

Current Status of Single Particle Imaging with X-ray Lasers

DOE PAGES

Sun, Zhibin; Fan, Jiadong; Li, Haoyuan; ...

2018-01-22

The advent of ultrafast X-ray free-electron lasers (XFELs) opens the tantalizing possibility of the atomic-resolution imaging of reproducible objects such as viruses, nanoparticles, single molecules, clusters, and perhaps biological cells, achieving a resolution for single particle imaging better than a few tens of nanometers. Improving upon this is a significant challenge which has been the focus of a global single particle imaging (SPI) initiative launched in December 2014 at the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, USA. A roadmap was outlined, and significant multi-disciplinary effort has since been devoted to work on the technical challenges of SPImore » such as radiation damage, beam characterization, beamline instrumentation and optics, sample preparation and delivery and algorithm development at multiple institutions involved in the SPI initiative. Currently, the SPI initiative has achieved 3D imaging of rice dwarf virus (RDV) and coliphage PR772 viruses at ~10 nm resolution by using soft X-ray FEL pulses at the Atomic Molecular and Optical (AMO) instrument of LCLS. Meanwhile, diffraction patterns with signal above noise up to the corner of the detector with a resolution of ~6 Ångström (Å) were also recorded with hard X-rays at the Coherent X-ray Imaging (CXI) instrument, also at LCLS. Achieving atomic resolution is truly a grand challenge and there is still a long way to go in light of recent developments in electron microscopy. However, the potential for studying dynamics at physiological conditions and capturing ultrafast biological, chemical and physical processes represents a tremendous potential application, attracting continued interest in pursuing further method development. In this paper, we give a brief introduction of SPI developments and look ahead to further method development.« less

Current Status of Single Particle Imaging with X-ray Lasers

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

Sun, Zhibin; Fan, Jiadong; Li, Haoyuan

The advent of ultrafast X-ray free-electron lasers (XFELs) opens the tantalizing possibility of the atomic-resolution imaging of reproducible objects such as viruses, nanoparticles, single molecules, clusters, and perhaps biological cells, achieving a resolution for single particle imaging better than a few tens of nanometers. Improving upon this is a significant challenge which has been the focus of a global single particle imaging (SPI) initiative launched in December 2014 at the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, USA. A roadmap was outlined, and significant multi-disciplinary effort has since been devoted to work on the technical challenges of SPImore » such as radiation damage, beam characterization, beamline instrumentation and optics, sample preparation and delivery and algorithm development at multiple institutions involved in the SPI initiative. Currently, the SPI initiative has achieved 3D imaging of rice dwarf virus (RDV) and coliphage PR772 viruses at ~10 nm resolution by using soft X-ray FEL pulses at the Atomic Molecular and Optical (AMO) instrument of LCLS. Meanwhile, diffraction patterns with signal above noise up to the corner of the detector with a resolution of ~6 Ångström (Å) were also recorded with hard X-rays at the Coherent X-ray Imaging (CXI) instrument, also at LCLS. Achieving atomic resolution is truly a grand challenge and there is still a long way to go in light of recent developments in electron microscopy. However, the potential for studying dynamics at physiological conditions and capturing ultrafast biological, chemical and physical processes represents a tremendous potential application, attracting continued interest in pursuing further method development. In this paper, we give a brief introduction of SPI developments and look ahead to further method development.« less

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

PubMed Central

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

2013-01-01

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

Simple and robust generation of ultrafast laser pulse trains using polarization-independent parallel-aligned thin films

NASA Astrophysics Data System (ADS)

Wang, Andong; Jiang, Lan; Li, Xiaowei; Wang, Zhi; Du, Kun; Lu, Yongfeng

2018-05-01

Ultrafast laser pulse temporal shaping has been widely applied in various important applications such as laser materials processing, coherent control of chemical reactions, and ultrafast imaging. However, temporal pulse shaping has been limited to only-in-lab technique due to the high cost, low damage threshold, and polarization dependence. Herein we propose a novel design of ultrafast laser pulse train generation device, which consists of multiple polarization-independent parallel-aligned thin films. Various pulse trains with controllable temporal profile can be generated flexibly by multi-reflections within the splitting films. Compared with other pulse train generation techniques, this method has advantages of compact structure, low cost, high damage threshold and polarization independence. These advantages endow it with high potential for broad utilization in ultrafast applications.

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

4D in vivo ultrafast ultrasound imaging using a row-column addressed matrix and coherently-compounded orthogonal plane waves

NASA Astrophysics Data System (ADS)

Flesch, M.; Pernot, M.; Provost, J.; Ferin, G.; Nguyen-Dinh, A.; Tanter, M.; Deffieux, T.

2017-06-01

4D ultrafast ultrasound imaging was recently shown using a 2D matrix (i.e. fully populated) connected to a 1024-channel ultrafast ultrasound scanner. In this study, we investigate the row-column addressing (RCA) matrix approach, which allows a reduction of independent channels from N  ×  N to N  +  N, with a dedicated beamforming strategy for ultrafast ultrasound imaging based on the coherent compounding of orthogonal plane wave (OPW). OPW is based on coherent compounding of plane wave transmissions in one direction with receive beamforming along the orthogonal direction and its orthogonal companion sequence. Such coherent recombination of complementary orthogonal sequences leads to the virtual transmit focusing in both directions which results into a final isotropic point spread function (PSF). In this study, a 32  ×  32 2D matrix array probe (1024 channels), centered at 5 MHz was considered. An RCA array, of same footprint with 32  +  32 elements (64 channels), was emulated by summing the elements either along a line or a column in software prior to beamforming. This approach allowed for the direct comparison of the 32  +  32 RCA scheme to the optimal fully sampled 32  ×  32 2D matrix configuration, which served as the gold standard. This approach was first studied through PSF simulations and then validated experimentally on a phantom consisting of anechoic cysts and echogenic wires. The contrast-to-noise ratio and the lateral resolution of the RCA approach were found to be approximately equal to half (in decibel) and twice the values, respectively, obtained when using the 2D matrix approach. Results in a Doppler phantom and the human humeral artery in vivo confirmed that ultrafast Doppler imaging can be achieved with reduced performances when compared against the equivalent 2D matrix. Volumetric anatomic Doppler rendering and voxel-based pulsed Doppler quantification are presented as well. OPW compound imaging using emulated RCA matrix can achieve a power Doppler with sufficient contrast to recover the vein shape and provides an accurate Doppler spectrum.

4D in vivo ultrafast ultrasound imaging using a row-column addressed matrix and coherently-compounded orthogonal plane waves.

PubMed

Flesch, M; Pernot, M; Provost, J; Ferin, G; Nguyen-Dinh, A; Tanter, M; Deffieux, T

2017-06-07

4D ultrafast ultrasound imaging was recently shown using a 2D matrix (i.e. fully populated) connected to a 1024-channel ultrafast ultrasound scanner. In this study, we investigate the row-column addressing (RCA) matrix approach, which allows a reduction of independent channels from N  ×  N to N  +  N, with a dedicated beamforming strategy for ultrafast ultrasound imaging based on the coherent compounding of orthogonal plane wave (OPW). OPW is based on coherent compounding of plane wave transmissions in one direction with receive beamforming along the orthogonal direction and its orthogonal companion sequence. Such coherent recombination of complementary orthogonal sequences leads to the virtual transmit focusing in both directions which results into a final isotropic point spread function (PSF). In this study, a 32  ×  32 2D matrix array probe (1024 channels), centered at 5 MHz was considered. An RCA array, of same footprint with 32  +  32 elements (64 channels), was emulated by summing the elements either along a line or a column in software prior to beamforming. This approach allowed for the direct comparison of the 32  +  32 RCA scheme to the optimal fully sampled 32  ×  32 2D matrix configuration, which served as the gold standard. This approach was first studied through PSF simulations and then validated experimentally on a phantom consisting of anechoic cysts and echogenic wires. The contrast-to-noise ratio and the lateral resolution of the RCA approach were found to be approximately equal to half (in decibel) and twice the values, respectively, obtained when using the 2D matrix approach. Results in a Doppler phantom and the human humeral artery in vivo confirmed that ultrafast Doppler imaging can be achieved with reduced performances when compared against the equivalent 2D matrix. Volumetric anatomic Doppler rendering and voxel-based pulsed Doppler quantification are presented as well. OPW compound imaging using emulated RCA matrix can achieve a power Doppler with sufficient contrast to recover the vein shape and provides an accurate Doppler spectrum.

The LAMP instrument at the Linac Coherent Light Source free-electron laser

NASA Astrophysics Data System (ADS)

Osipov, Timur; Bostedt, Christoph; Castagna, J.-C.; Ferguson, Ken R.; Bucher, Maximilian; Montero, Sebastian C.; Swiggers, Michele L.; Obaid, Razib; Rolles, Daniel; Rudenko, Artem; Bozek, John D.; Berrah, Nora

2018-03-01

The Laser Applications in Materials Processing (LAMP) instrument is a new end-station for soft X-ray imaging, high-field physics, and ultrafast X-ray science experiments that is available to users at the Linac Coherent Light Source (LCLS) free-electron laser. While the instrument resides in the Atomic, Molecular and Optical science hutch, its components can be used at any LCLS beamline. The end-station has a modular design that provides high flexibility in order to meet user-defined experimental requirements and specifications. The ultra-high-vacuum environment supports different sample delivery systems, including pulsed and continuous atomic, molecular, and cluster jets; liquid and aerosols jets; and effusive metal vapor beams. It also houses movable, large-format, high-speed pnCCD X-ray detectors for detecting scattered and fluorescent photons. Multiple charged-particle spectrometer options are compatible with the LAMP chamber, including a double-sided spectrometer for simultaneous and even coincident measurements of electrons, ions, and photons produced by the interaction of the high-intensity X-ray beam with the various samples. Here we describe the design and capabilities of the spectrometers along with some general aspects of the LAMP chamber and show some results from the initial instrument commissioning.

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.

Strategies to improve phase-stability of ultrafast swept source optical coherence tomography for single shot imaging of transient mechanical waves at 16 kHz frame rate

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

Song, Shaozhen; Wei, Wei; Hsieh, Bao-Yu

We present single-shot phase-sensitive imaging of propagating mechanical waves within tissue, enabled by an ultrafast optical coherence tomography (OCT) system powered by a 1.628 MHz Fourier domain mode-locked (FDML) swept laser source. We propose a practical strategy for phase-sensitive measurement by comparing the phases between adjacent OCT B-scans, where the B-scan contains a number of A-scans equaling an integer number of FDML buffers. With this approach, we show that micro-strain fields can be mapped with ∼3.0 nm sensitivity at ∼16 000 fps. The system's capabilities are demonstrated on porcine cornea by imaging mechanical wave propagation launched by a pulsed UV laser beam, promisingmore » non-contact, real-time, and high-resolution optical coherence elastography.« less

Conformational Dynamics Guides Coherent Exciton Migration in Conjugated Polymer Materials: First-Principles Quantum Dynamical Study

NASA Astrophysics Data System (ADS)

Binder, Robert; Lauvergnat, David; Burghardt, Irene

2018-06-01

We report on high-dimensional quantum dynamical simulations of photoinduced exciton migration in a single-chain oligothiophene segment, in view of elucidating the controversial nature of the elementary exciton transport steps in semiconducting polymers. A novel first-principles parametrized Frenkel J aggregate Hamiltonian is employed that goes significantly beyond the standard Frenkel-Holstein Hamiltonian. Departing from a nonequilibrium state created by photoexcitation, these simulations provide evidence of an ultrafast two-timescale process at low temperatures, involving exciton-polaron formation within tens of femtoseconds (fs), followed by torsional relaxation on an ˜400 fs timescale. The second step is the driving force for exciton migration, as initial conjugation breaks are removed by dynamical planarization. The quantum coherent nature of the elementary exciton migration step is consistent with experimental observations highlighting the correlated and vibrationally coherent nature of the dynamics on ultrafast timescales.

Tracking the coherent generation of polaron pairs in conjugated polymers

NASA Astrophysics Data System (ADS)

de Sio, Antonietta; Troiani, Filippo; Maiuri, Margherita; Réhault, Julien; Sommer, Ephraim; Lim, James; Huelga, Susana F.; Plenio, Martin B.; Rozzi, Carlo Andrea; Cerullo, Giulio; Molinari, Elisa; Lienau, Christoph

2016-12-01

The optical excitation of organic semiconductors not only generates charge-neutral electron-hole pairs (excitons), but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence at room temperature. The measured two-dimensional spectra show pronounced peak splittings revealing that the elementary optical excitations of this polymer are hybridized exciton-polaron-pairs, strongly coupled to a dominant underdamped vibrational mode. Coherent vibronic coupling induces ultrafast polaron pair formation, accelerates the charge separation dynamics and makes it insensitive to disorder. These findings open up new perspectives for tailoring light-to-current conversion in organic materials.

Conformational Dynamics Guides Coherent Exciton Migration in Conjugated Polymer Materials: First-Principles Quantum Dynamical Study.

PubMed

Binder, Robert; Lauvergnat, David; Burghardt, Irene

2018-06-01

We report on high-dimensional quantum dynamical simulations of photoinduced exciton migration in a single-chain oligothiophene segment, in view of elucidating the controversial nature of the elementary exciton transport steps in semiconducting polymers. A novel first-principles parametrized Frenkel J aggregate Hamiltonian is employed that goes significantly beyond the standard Frenkel-Holstein Hamiltonian. Departing from a nonequilibrium state created by photoexcitation, these simulations provide evidence of an ultrafast two-timescale process at low temperatures, involving exciton-polaron formation within tens of femtoseconds (fs), followed by torsional relaxation on an ∼400  fs timescale. The second step is the driving force for exciton migration, as initial conjugation breaks are removed by dynamical planarization. The quantum coherent nature of the elementary exciton migration step is consistent with experimental observations highlighting the correlated and vibrationally coherent nature of the dynamics on ultrafast timescales.

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

NASA Astrophysics Data System (ADS)

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

2018-06-01

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

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

Direct characterization of photoinduced lattice dynamics in BaFe 2As 2

DOE PAGES

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

2015-06-08

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

Direct characterization of photoinduced lattice dynamics in BaFe2As2

PubMed Central

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

2015-01-01

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

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

PubMed

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

2018-05-09

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

Coherent Soft X-ray Diffraction Imaging of Coliphage PR772 at the Linac Coherent Light Source

DOE Data Explorer

Reddy, Hemanth, K.N.

2017-01-05

A dataset of coherent soft X-ray diffraction images of Coliphage PR772 virus, collected at the Atomic Molecular Optics (AMO) beamline with pnCCD detectors in the LAMP instrument at the Linac Coherent Light Source.

Quantum Nuclear Dynamics Pumped and Probed by Ultrafast Polarization Controlled Steering of a Coherent Electronic State in LiH.

PubMed

Nikodem, Astrid; Levine, R D; Remacle, F

2016-05-19

The quantum wave packet dynamics following a coherent electronic excitation of LiH by an ultrashort, polarized, strong one-cycle infrared optical pulse is computed on several electronic states using a grid method. The coupling to the strong field of the pump and the probe pulses is included in the Hamiltonian used to solve the time-dependent Schrodinger equation. The polarization of the pump pulse allows us to control the localization in time and in space of the nonequilibrium coherent electronic motion and the subsequent nuclear dynamics. We show that transient absorption, resulting from the interaction of the total molecular dipole with the electric fields of the pump and the probe, is a very versatile probe of the different time scales of the vibronic dynamics. It allows probing both the ultrashort, femtosecond time scale of the electronic coherences as well as the longer dozens of femtoseconds time scales of the nuclear motion on the excited electronic states. The ultrafast beatings of the electronic coherences in space and in time are shown to be modulated by the different periods of the nuclear motion.

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

Anomalous Phase Change in [(GeTe)2/(Sb2Te3)]20 Superlattice Observed by Coherent Phonon Spectroscopy

NASA Astrophysics Data System (ADS)

Makino, K.; Saito, Y.; Mitrofanov, K.; Tominaga, J.; Kolobov, A. V.; Nakano, T.; Fons, P.; Hase, M.

The temperature-dependent ultrafast coherent phonon dynamics of topological (GeTe)2/(Sb2Te3) super lattice phase change memory material was investigated. By comparing with Ge-Sb-Te alloy, a clear contrast suggesting the unique phase change behavior was found.

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.

Ultrafast High Harmonic, Soft X-Ray Probing of Molecular Dynamics

DTIC Science & Technology

2013-04-30

590 L/s scroll pump and a titanium sublimation pump . A TOF-PES has been designed and constructed to analyze the energy of the photoelectrons...are studied using the quasi-continuous vacuum ultraviolet light of the Advanced Light Source at Lawrence Berkeley National Laboratory. The molecular...34), the method of high order harmonic generation of ultrashort vacuum ultraviolet pulses was used to investigate molecular photodissociation, ultrafast

Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite

DOE PAGES

Luo, Liang; Men, Long; Liu, Zhaoyu; ...

2017-06-01

How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics. Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system. Furthermore we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot statemore » cooling processes. The nearly ~1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ~13.5 meV in perovskites are distinct from conventional photovoltaic semiconductors. In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices.« less

Evidence for carrier localization in the pseudogap state of cuprate superconductors from coherent quench experiments

PubMed Central

Madan, I.; Kurosawa, T.; Toda, Y.; Oda, M.; Mertelj, T.; Mihailovic, D.

2015-01-01

A ‘pseudogap' was introduced by Mott to describe a state of matter that has a minimum in the density of states at the Fermi level, deep enough for states to become localized. It can arise either from Coulomb repulsion between electrons, and/or incipient charge or spin order. Here we employ ultrafast spectroscopy to study dynamical properties of the normal to pseudogap state transition in the prototype high-temperature superconductor Bi2Sr2CaCu2O8+δ. We perform a systematic temperature and doping dependence study of the pseudogap photodestruction and recovery in coherent quench experiments, revealing marked absence of critical behaviour of the elementary excitations, which implies an absence of collective electronic ordering beyond a few coherence lengths on short timescales. The data imply ultrafast carrier localization into a textured polaronic state arising from a competing Coulomb interaction and lattice strain, enhanced by a Fermi surface instability. PMID:25891310

Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite

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

Luo, Liang; Men, Long; Liu, Zhaoyu

How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics. Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system. Furthermore we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot statemore » cooling processes. The nearly ~1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ~13.5 meV in perovskites are distinct from conventional photovoltaic semiconductors. In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices.« less

Ultrafast creation of large Schrödinger cat states of an atom.

PubMed

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

2017-09-26

Mesoscopic quantum superpositions, or Schrödinger cat states, are widely studied for fundamental investigations of quantum measurement and decoherence as well as applications in sensing and quantum information science. The generation and maintenance of such states relies upon a balance between efficient external coherent control of the system and sufficient isolation from the environment. Here we create a variety of cat states of a single trapped atom's motion in a harmonic oscillator using ultrafast laser pulses. These pulses produce high fidelity impulsive forces that separate the atom into widely separated positions, without restrictions that typically limit the speed of the interaction or the size and complexity of the resulting motional superposition. This allows us to quickly generate and measure cat states larger than previously achieved in a harmonic oscillator, and create complex multi-component superposition states in atoms.Generation of mesoscopic quantum superpositions requires both reliable coherent control and isolation from the environment. Here, the authors succeed in creating a variety of cat states of a single trapped atom, mapping spin superpositions into spatial superpositions using ultrafast laser pulses.

Uncovering Highly-Excited State Mixing in Acetone Using Ultrafast VUV Pulses and Coincidence Imaging Techniques

DOE PAGES

Couch, David E.; Kapteyn, Henry C.; Murnane, Margaret M.; ...

2017-03-17

Here, understanding the ultrafast dynamics of highly-excited electronic states of small molecules is critical for a better understanding of atmospheric and astrophysical processes, as well as for designing coherent control strategies for manipulating chemical dynamics. In highly excited states, nonadiabatic coupling, electron-electron interactions, and the high density of states govern dynamics. However, these states are computationally and experimentally challenging to access. Fortunately, new sources of ultrafast vacuum ultraviolet pulses, in combination with electron-ion coincidence spectroscopies, provide new tools to unravel the complex electronic landscape. Here we report time-resolved photoelectron-photoion coincidence experiments using 8 eV pump photons to study the highlymore » excited states of acetone. We uncover for the first time direct evidence that the resulting excited state consists of a mixture of both n y → 3p and π → π* character, which decays with a time constant of 330 fs. In the future, this approach can inform models of VUV photochemistry and aid in designing coherent control strategies for manipulating chemical reactions.« less

Uncovering Highly-Excited State Mixing in Acetone Using Ultrafast VUV Pulses and Coincidence Imaging Techniques

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

Couch, David E.; Kapteyn, Henry C.; Murnane, Margaret M.

Here, understanding the ultrafast dynamics of highly-excited electronic states of small molecules is critical for a better understanding of atmospheric and astrophysical processes, as well as for designing coherent control strategies for manipulating chemical dynamics. In highly excited states, nonadiabatic coupling, electron-electron interactions, and the high density of states govern dynamics. However, these states are computationally and experimentally challenging to access. Fortunately, new sources of ultrafast vacuum ultraviolet pulses, in combination with electron-ion coincidence spectroscopies, provide new tools to unravel the complex electronic landscape. Here we report time-resolved photoelectron-photoion coincidence experiments using 8 eV pump photons to study the highlymore » excited states of acetone. We uncover for the first time direct evidence that the resulting excited state consists of a mixture of both n y → 3p and π → π* character, which decays with a time constant of 330 fs. In the future, this approach can inform models of VUV photochemistry and aid in designing coherent control strategies for manipulating chemical reactions.« less

The LAMP instrument at the Linac Coherent Light Source free-electron laser

DOE PAGES

Osipov, Timur; Bostedt, Christoph; Castagna, J. -C.; ...

2018-03-23

The Laser Applications in Materials Processing (LAMP) instrument is a new end-station for soft X-ray imaging, high-field physics, and ultrafast X-ray science experiments that is available to users at the Linac Coherent Light Source (LCLS) free-electron laser. While the instrument resides in the Atomic, Molecular and Optical science hutch, its components can be used at any LCLS beamline. The end-station has a modular design that provides high flexibility in order to meet user-defined experimental requirements and specifications. The ultra-high-vacuum environment supports different sample delivery systems, including pulsed and continuous atomic, molecular, and cluster jets; liquid and aerosols jets; and effusivemore » metal vapor beams. It also houses movable, large-format, high-speed pnCCD X-ray detectors for detecting scattered and fluorescent photons. Multiple charged-particle spectrometer options are compatible with the LAMP chamber, including a double-sided spectrometer for simultaneous and even coincident measurements of electrons, ions, and photons produced by the interaction of the high-intensity X-ray beam with the various samples. Here in this paper we describe the design and capabilities of the spectrometers along with some general aspects of the LAMP chamber and show some results from the initial instrument commissioning.« less

The LAMP instrument at the Linac Coherent Light Source free-electron laser

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

Osipov, Timur; Bostedt, Christoph; Castagna, J. -C.

The Laser Applications in Materials Processing (LAMP) instrument is a new end-station for soft X-ray imaging, high-field physics, and ultrafast X-ray science experiments that is available to users at the Linac Coherent Light Source (LCLS) free-electron laser. While the instrument resides in the Atomic, Molecular and Optical science hutch, its components can be used at any LCLS beamline. The end-station has a modular design that provides high flexibility in order to meet user-defined experimental requirements and specifications. The ultra-high-vacuum environment supports different sample delivery systems, including pulsed and continuous atomic, molecular, and cluster jets; liquid and aerosols jets; and effusivemore » metal vapor beams. It also houses movable, large-format, high-speed pnCCD X-ray detectors for detecting scattered and fluorescent photons. Multiple charged-particle spectrometer options are compatible with the LAMP chamber, including a double-sided spectrometer for simultaneous and even coincident measurements of electrons, ions, and photons produced by the interaction of the high-intensity X-ray beam with the various samples. Here in this paper we describe the design and capabilities of the spectrometers along with some general aspects of the LAMP chamber and show some results from the initial instrument commissioning.« less

Direct comparison of shot-to-shot noise performance of all normal dispersion and anomalous dispersion supercontinuum pumped with sub-picosecond pulse fiber-based laser

PubMed Central

Klimczak, Mariusz; Soboń, Grzegorz; Kasztelanic, Rafał; Abramski, Krzysztof M.; Buczyński, Ryszard

2016-01-01

Coherence of supercontinuum sources is critical for applications involving characterization of ultrafast or rarely occurring phenomena. With the demonstrated spectral coverage of supercontinuum extending from near-infrared to over 10 μm in a single nonlinear fiber, there has been a clear push for the bandwidth rather than for attempting to optimize the dynamic properties of the generated spectrum. In this work we provide an experimental assessment of the shot-to-shot noise performance of supercontinuum generation in two types of soft glass photonic crystal fibers. Phase coherence and intensity fluctuations are compared for the cases of an anomalous dispersion-pumped fiber and an all-normal dispersion fiber. With the use of the dispersive Fourier transformation method, we demonstrate that a factor of 100 improvement in signal-to-noise ratio is achieved in the normal-dispersion over anomalous dispersion-pumped fiber for 390 fs long pump pulses. A double-clad design of the photonic lattice of the fiber is further postulated to enable a pump-related seeding mechanism of normal-dispersion supercontinuum broadening under sub-picosecond pumping, which is otherwise known for similar noise characteristics as modulation instability driven, soliton-based spectra. PMID:26759188

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

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

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

2016-03-14

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

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

NASA Astrophysics Data System (ADS)

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

2016-03-01

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

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.

Ultrafast dynamics of quasiparticles and coherent acoustic phonons in slightly underdoped (BaK)Fe2As2

PubMed Central

Lin, Kung-Hsuan; Wang, Kuan-Jen; Chang, Chung-Chieh; Wen, Yu-Chieh; Lv, Bing; Chu, Ching-Wu; Wu, Maw-Kuen

2016-01-01

We have utilized ultrafast optical spectroscopy to study carrier dynamics in slightly underdoped (BaK)Fe2As2 crystals without magnetic transition. The photoelastic signals due to coherent acoustic phonons have been quantitatively investigated. According to our temperature-dependent results, we found that the relaxation component of superconducting quasiparticles persisted from the superconducting state up to at least 70 K in the normal state. Our findings suggest that the pseudogaplike feature in the normal state is possibly the precursor of superconductivity. We also highlight that the pseudogap feature of K-doped BaFe2As2 is different from that of other iron-based superconductors, including Co-doped or P-doped BaFe2As2. PMID:27180873

Evidence of an Improper Displacive Phase Transition in Cd2 Re2 O7 via Time-Resolved Coherent Phonon Spectroscopy

NASA Astrophysics Data System (ADS)

Harter, J. W.; Kennes, D. M.; Chu, H.; de la Torre, A.; Zhao, Z. Y.; Yan, J.-Q.; Mandrus, D. G.; Millis, A. J.; Hsieh, D.

2018-01-01

We have used a combination of ultrafast coherent phonon spectroscopy, ultrafast thermometry, and time-dependent Landau theory to study the inversion symmetry breaking phase transition at Tc=200 K in the strongly spin-orbit coupled correlated metal Cd2 Re2 O7 . We establish that the structural distortion at Tc is a secondary effect through the absence of any softening of its associated phonon mode, which supports a purely electronically driven mechanism. However, the phonon lifetime exhibits an anomalously strong temperature dependence that decreases linearly to zero near Tc. We show that this behavior naturally explains the spurious appearance of phonon softening in previous Raman spectroscopy experiments and should be a prevalent feature of correlated electron systems with linearly coupled order parameters.

Direct Imaging of Frenkel Exciton Transport by Ultrafast Microscopy.

PubMed

Zhu, Tong; Wan, Yan; Huang, Libai

2017-07-18

Long-range transport of Frenkel excitons is crucial for achieving efficient molecular-based solar energy harvesting. Understanding of exciton transport mechanisms is important for designing materials for solar energy applications. One major bottleneck in unraveling of exciton transport mechanisms is the lack of direct measurements to provide information in both spatial and temporal domains, imposed by the combination of fast energy transfer (typically ≤1 ps) and short exciton diffusion lengths (typically ≤100 nm). This challenge requires developing experimental tools to directly characterize excitation energy transport, and thus facilitate the elucidation of mechanisms. To address this challenge, we have employed ultrafast transient absorption microscopy (TAM) as a means to directly image exciton transport with ∼200 fs time resolution and ∼50 nm spatial precision. By mapping population in spatial and temporal domains, such approach has unraveled otherwise obscured information and provided important parameters for testing exciton transport models. In this Account, we discuss the recent progress in imaging Frenkel exciton migration in molecular crystals and aggregates by ultrafast microscopy. First, we establish the validity of the TAM methods by imaging singlet and triplet exciton transport in a series of polyacene single crystals that undergo singlet fission. A new singlet-mediated triplet transport pathway has been revealed by TAM, resulting from the equilibrium between triplet and singlet exciton populations. Such enhancement of triplet exciton transport enables triplet excitons to migrate as singlet excitons and leads to orders of magnitude faster apparent triplet exciton diffusion rate in the picosecond and nanosecond time scales, favorable for solar cell applications. Next we discuss how information obtained by ultrafast microscopy can evaluate coherent effects in exciton transport. We use tubular molecular aggregates that could support large exciton delocalization sizes as a model system. The initial experiments measure exciton diffusion constants of 3-6 cm 2 s -1 , 3-5 times higher than the incoherent limit predicted by theory, suggesting that coherent effects play a role. In summary, combining ultrafast spectroscopic methods with microscopic techniques provides a direct approach for obtaining important parameters to unravel the underlying exciton transport mechanisms in molecular solids. We discuss future directions to bridge the gap in understanding of fundamental energy transfer theories to include coherent and incoherent effects. We are still in the infancy of ultrafast microscopy, and the vast potential is not limited to the systems discussed in this Account.

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.

10-fs-level synchronization of photocathode laser with RF-oscillator for ultrafast electron and X-ray sources

PubMed Central

Yang, Heewon; Han, Byungheon; Shin, Junho; Hou, Dong; Chung, Hayun; Baek, In Hyung; Jeong, Young Uk; Kim, Jungwon

2017-01-01

Ultrafast electron-based coherent radiation sources, such as free-electron lasers (FELs), ultrafast electron diffraction (UED) and Thomson-scattering sources, are becoming more important sources in today’s ultrafast science. Photocathode laser is an indispensable common subsystem in these sources that generates ultrafast electron pulses. To fully exploit the potentials of these sources, especially for pump-probe experiments, it is important to achieve high-precision synchronization between the photocathode laser and radio-frequency (RF) sources that manipulate electron pulses. So far, most of precision laser-RF synchronization has been achieved by using specially designed low-noise Er-fibre lasers at telecommunication wavelength. Here we show a modular method that achieves long-term (>1 day) stable 10-fs-level synchronization between a commercial 79.33-MHz Ti:sapphire laser oscillator and an S-band (2.856-GHz) RF oscillator. This is an important first step toward a photocathode laser-based femtosecond RF timing and synchronization system that is suitable for various small- to mid-scale ultrafast X-ray and electron sources. PMID:28067288

10-fs-level synchronization of photocathode laser with RF-oscillator for ultrafast electron and X-ray sources

NASA Astrophysics Data System (ADS)

Yang, Heewon; Han, Byungheon; Shin, Junho; Hou, Dong; Chung, Hayun; Baek, In Hyung; Jeong, Young Uk; Kim, Jungwon

2017-01-01

Ultrafast electron-based coherent radiation sources, such as free-electron lasers (FELs), ultrafast electron diffraction (UED) and Thomson-scattering sources, are becoming more important sources in today’s ultrafast science. Photocathode laser is an indispensable common subsystem in these sources that generates ultrafast electron pulses. To fully exploit the potentials of these sources, especially for pump-probe experiments, it is important to achieve high-precision synchronization between the photocathode laser and radio-frequency (RF) sources that manipulate electron pulses. So far, most of precision laser-RF synchronization has been achieved by using specially designed low-noise Er-fibre lasers at telecommunication wavelength. Here we show a modular method that achieves long-term (>1 day) stable 10-fs-level synchronization between a commercial 79.33-MHz Ti:sapphire laser oscillator and an S-band (2.856-GHz) RF oscillator. This is an important first step toward a photocathode laser-based femtosecond RF timing and synchronization system that is suitable for various small- to mid-scale ultrafast X-ray and electron sources.

Ultrafast Photoinduced Multimode Antiferromagnetic Spin Dynamics in Exchange-Coupled Fe/RFeO3 (R = Er or Dy) Heterostructures.

PubMed

Tang, Jin; Ke, Yajiao; He, Wei; Zhang, Xiangqun; Zhang, Wei; Li, Na; Zhang, Yongsheng; Li, Yan; Cheng, Zhaohua

2018-05-25

Antiferromagnetic spin dynamics is important for both fundamental and applied antiferromagnetic spintronic devices; however, it is rarely explored by external fields because of the strong exchange interaction in antiferromagnetic materials. Here, the photoinduced excitation of ultrafast antiferromagnetic spin dynamics is achieved by capping antiferromagnetic RFeO 3 (R = Er or Dy) with an exchange-coupled ferromagnetic Fe film. Compared with antiferromagnetic spin dynamics of bare RFeO 3 orthoferrite single crystals, which can be triggered effectively by ultrafast laser heating just below the phase transition temperature, the ultrafast photoinduced multimode antiferromagnetic spin dynamic modes, for exchange-coupled Fe/RFeO 3 heterostructures, including quasiferromagnetic resonance, impurity, coherent phonon, and quasiantiferromagnetic modes, are observed in a temperature range of 10-300 K. These experimental results not only offer an effective means to trigger ultrafast antiferromagnetic spin dynamics of rare-earth orthoferrites, but also shed light on the ultrafast manipulation of antiferromagnetic magnetization in Fe/RFeO 3 heterostructures. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

10-fs-level synchronization of photocathode laser with RF-oscillator for ultrafast electron and X-ray sources.

PubMed

Yang, Heewon; Han, Byungheon; Shin, Junho; Hou, Dong; Chung, Hayun; Baek, In Hyung; Jeong, Young Uk; Kim, Jungwon

2017-01-09

Ultrafast electron-based coherent radiation sources, such as free-electron lasers (FELs), ultrafast electron diffraction (UED) and Thomson-scattering sources, are becoming more important sources in today's ultrafast science. Photocathode laser is an indispensable common subsystem in these sources that generates ultrafast electron pulses. To fully exploit the potentials of these sources, especially for pump-probe experiments, it is important to achieve high-precision synchronization between the photocathode laser and radio-frequency (RF) sources that manipulate electron pulses. So far, most of precision laser-RF synchronization has been achieved by using specially designed low-noise Er-fibre lasers at telecommunication wavelength. Here we show a modular method that achieves long-term (>1 day) stable 10-fs-level synchronization between a commercial 79.33-MHz Ti:sapphire laser oscillator and an S-band (2.856-GHz) RF oscillator. This is an important first step toward a photocathode laser-based femtosecond RF timing and synchronization system that is suitable for various small- to mid-scale ultrafast X-ray and electron sources.

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

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.

Testing ultrafast mode-locking at microhertz relative optical linewidth.

PubMed

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

2009-01-19

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

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

DTIC Science & Technology

2008-03-01

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

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.

(DURIP 09) Ultrafast Laser System for Coherent Anti-Stokes Raman Scattering Measurements at Data Rates of 5 kHz

DTIC Science & Technology

2010-08-22

tunable beam that will be used for the pump radiation in the femtosecond coherent anti-Stokes Raman scattering ( CARS ) measurements. This system has been...beam that will be used for the pump radiation in the femtosecond coherent anti-Stokes Raman scattering ( CARS ) measurements. This system has been... CARS ) spectroscopy. Fs CARS offers some significant potential advantages compared with nanosecond (ns) CARS , i.e., CARS as usually performed with ns

Synchronous Measurement of Ultrafast Anisotropy Decay of the B850 in Bacterial LH2 Complex

NASA Astrophysics Data System (ADS)

Wang, Yun-Peng; Du, Lu-Chao; Zhu, Gang-Bei; Wang, Zhuan; Weng, Yu-Xiang

2015-02-01

Ultrafast anisotropic decay is a prominent parameter revealing ultrafast energy and electron transfer; however, it is difficult to be determined reliably owing to the requirement of a simultaneous availability of the parallel and perpendicular polarized decay kinetics. Nowadays, any measurement of anisotropic decay is a kind of approach to the exact simultaneity. Here we report a novel method for a synchronous ultrafast anisotropy decay measurement, which can well determine the anisotropy, even at a very early time, as the rising phase of the excitation laser pulse. The anisotropic decay of the B850 in bacterial light harvesting antenna complex LH2 of Rhodobacter sphaeroides in solution at room temperature with coherent excitation is detected by this method, which shows a polarization response time of 30 fs, and the energy transfer from the initial excitation to the bacteriochlorophylls in B850 ring takes about 70 fs. The anisotropic decay that is probed at the red side of the absorption spectrum, such as 880 nm, has an initial value of 0.4, corresponding to simulated emission, while the blue side with an anisotropy of 0.1 contributes to the ground-state bleaching. Our results show that the coherent excitation covering the whole ring might not be realized owing to the symmetry breaking of LH2: from C9 symmetry in membrane to C2 symmetry in solution.

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 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.

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

NASA Astrophysics Data System (ADS)

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

2017-03-01

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

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

Collapse of superconductivity in cuprates via ultrafast quenching of phase coherence

DOE PAGES

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

2018-04-02

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

Collapse of superconductivity in cuprates via ultrafast quenching of phase coherence

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

Hotspot-mediated non-dissipative and ultrafast plasmon passage

NASA Astrophysics Data System (ADS)

Roller, Eva-Maria; Besteiro, Lucas V.; Pupp, Claudia; Khorashad, Larousse Khosravi; Govorov, Alexander O.; Liedl, Tim

2017-08-01

Plasmonic nanoparticles hold great promise as photon handling elements and as channels for coherent transfer of energy and information in future all-optical computing devices. Coherent energy oscillations between two spatially separated plasmonic entities via a virtual middle state exemplify electron-based population transfer, but their realization requires precise nanoscale positioning of heterogeneous particles. Here, we show the assembly and optical analysis of a triple-particle system consisting of two gold nanoparticles with an inter-spaced silver island. We observe strong plasmonic coupling between the spatially separated gold particles, mediated by the connecting silver particle, with almost no dissipation of energy. As the excitation energy of the silver island exceeds that of the gold particles, only quasi-occupation of the silver transfer channel is possible. We describe this effect both with exact classical electrodynamic modelling and qualitative quantum-mechanical calculations. We identify the formation of strong hotspots between all particles as the main mechanism for the lossless coupling and thus coherent ultrafast energy transfer between the remote partners. Our findings could prove useful for quantum gate operations, as well as for classical charge and information transfer processes.

Coherent energy scale revealed by ultrafast dynamics of UX3 (X = Al, Sn, Ga) single crystals

NASA Astrophysics Data System (ADS)

Nair, Saritha K.; Zhu, J.-X.; Sarrao, J. L.; Taylor, A. J.; Chia, Elbert E. M.

2012-09-01

The temperature dependence of relaxation dynamics of UX3 (X = Al, Ga, Sn) compounds is studied using the time-resolved pump-probe technique in reflectance geometry. For UGa3, our data are consistent with the formation of a spin density wave gap as evidenced from the quasidivergence of the relaxation time τ near the Néel temperature TN. For UAl3 and USn3, the relaxation dynamics shows a change from single-exponential to two-exponential behavior below a particular temperature, suggestive of coherence formation of the 5f electrons with the conduction band electrons. This particular temperature can be attributed to the spin fluctuation temperature Tsf, a measure of the strength of Kondo coherence. Our Tsf is consistent with other data such as resistivity and susceptibility measurements. The temperature dependence of the relaxation amplitude and time of UAl3 and USn3 were also fitted by the Rothwarf-Taylor model. Our results show that ultrafast optical spectroscopy is sensitive to c-f Kondo hybridization in the f-electron systems.

The Linac Coherent Light Source: Recent Developments and Future Plans

DOE PAGES

Schoenlein, R. W.; Boutet, S.; Minitti, M. P.; ...

2017-08-18

The development of X-ray free-electron lasers (XFELs) has launched a new era in X-ray science by providing ultrafast coherent X-ray pulses with a peak brightness that is approximately one billion times higher than previous X-ray sources. The Linac Coherent Light Source (LCLS) facility at the SLAC National Accelerator Laboratory, the world’s first hard X-ray FEL, has already demonstrated a tremendous scientific impact across broad areas of science. Here in this paper, a few of the more recent representative highlights from LCLS are presented in the areas of atomic, molecular, and optical science; chemistry; condensed matter physics; matter in extreme conditions;more » and biology. This paper also outlines the near term upgrade (LCLS-II) and motivating science opportunities for ultrafast X-rays in the 0.25–5 keV range at repetition rates up to 1 MHz. Future plans to extend the X-ray energy reach to beyond 13 keV (<1 Å) at high repetition rate (LCLS-II-HE) are envisioned, motivated by compelling new science of structural dynamics at the atomic scale.« less

Collapse of superconductivity in cuprates via ultrafast quenching of phase coherence

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

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

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

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.

Depth-Dependent Defect Studies Using Coherent Acoustic Phonons

DTIC Science & Technology

2014-09-29

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

Numerical Simulation of Ultra-Fast Pulse Propagation in Two-Photon Absorbing Medium

DTIC Science & Technology

2011-08-01

physical problems including coherent- and incoherent regimes of optical power limiting, saturation, CEP effects, soliton formation etc. It can be also...coherent- and incoherent regimes of optical power limiting, saturation, CEP effects, electromagnetically induced transparency, soliton formation etc...experimental data ( dark blue); Upper panel - 1PA spectrum; Lower panel - 2PA cross section spectrum. The parameter values used are shown in Table 1. 10

Intensity correlation measurement system by picosecond single shot soft x-ray laser.

PubMed

Kishimoto, Maki; Namikawa, Kazumichi; Sukegawa, Kouta; Yamatani, Hiroshi; Hasegawa, Noboru; Tanaka, Momoko

2010-01-01

We developed a new soft x-ray speckle intensity correlation spectroscopy system by use of a single shot high brilliant plasma soft x-ray laser. The plasma soft x-ray laser is characterized by several picoseconds in pulse width, more than 90% special coherence, and 10(11) soft x-ray photons within a single pulse. We developed a Michelson type delay pulse generator using a soft x-ray beam splitter to measure the intensity correlation of x-ray speckles from materials and succeeded in generating double coherent x-ray pulses with picosecond delay times. Moreover, we employed a high-speed soft x-ray streak camera for the picosecond time-resolved measurement of x-ray speckles caused by double coherent x-ray pulse illumination. We performed the x-ray speckle intensity correlation measurements for probing the relaxation phenomena of polarizations in polarization clusters in the paraelectric phase of the ferroelectric material BaTiO(3) near its Curie temperature and verified its performance.

PREFACE: Ultrafast biophotonics Ultrafast biophotonics

NASA Astrophysics Data System (ADS)

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

2010-08-01

The use of light to explore biology can be traced to the first observations of tissue made with early microscopes in the mid-seventeenth century, and has today evolved into the discipline which we now know as biophotonics. This field encompasses a diverse range of activities, each of which shares the common theme of exploiting the interaction of light with biological material. With the rapid advancement of ultrafast optical technologies over the last few decades, ultrafast lasers have increasingly found applications in biophotonics, to the extent that the distinctive new field of ultrafast biophotonics has now emerged, where robust turnkey ultrafast laser systems are facilitating cutting-edge studies in the life sciences to take place in everyday laboratories. The broad spectral bandwidths, precision timing resolution, low coherence and high peak powers of ultrafast optical pulses provide unique opportunities for imaging and manipulating biological systems. Time-resolved studies of bio-molecular dynamics exploit the short pulse durations from such lasers, while other applications such as optical coherence tomography benefit from the broad optical bandwidths possible by using super-continuum generation and additionally allowing for high speed imaging with speeds as high as 47 000 scans per second. Continuing progress in laser-system technology is accelerating the adoption of ultrafast techniques across the life sciences, both in research laboratories and in clinical applications, such as laser-assisted in situ keratomileusis (LASIK) eye surgery. Revolutionizing the field of optical microscopy, two-photon excitation fluorescence (TPEF) microscopy has enabled higher spatial resolution with improved depth penetration into biological specimens. Advantages of this nonlinear optical process include: reduced photo-interactions, allowing for extensive imaging time periods; simultaneously exciting multiple fluorescent molecules with only one excitation wavelength; and reduced chromatic aberration effects. These extensive advantages have led to further exploration of nonlinear processes including second-harmonic generation (SHG) microscopy and third-harmonic generation (THG) microscopy. Second-harmonic generation has provided biologists with an extremely powerful tool for generating contrast in biological imaging, with the additional benefit of non-invasive three-dimensional imaging. The recent popularity of THG microscopy is largely due to the fact that three-dimensional imaging is achievable without the need for any labels, but rather relying on the intrinsic properties of the biological specimen itself. This optical nonlinear technique has attracted much attention recently from the biological community due to its non-invasive capabilities. Users of ultrafast lasers in the biological and medical fields are becoming a fast-growing community, employing pulse-shaping microscopy, resolution-enhancing microscopy techniques, linear and nonlinear micro-spectroscopy, functional deep-tissue imaging, optical coherence tomography, nonlinear fluorescence microscopy, molecular imaging and control, harmonic microscopy and femtosecond lifetime imaging, for cutting-edge research concerning the interaction of light with biological dynamics. The adaptability of ultrafast lasers to interact with a large array of materials through nonlinear excitation has enabled precise control of laser fluence allowing for highly localized material interactions, permitting micro-structured fabricated surfaces. The resultant multi-dimensional fabricated micro-structures are capable of replicating and/or manipulating microenvironments for controlled cell biology. In this special issue of Journal of Optics readers have a chance to view a collection of new contributions to the growing research field of ultrafast biophotonics. They are presented with recent advances in ultrafast technology applied to biological and medical investigations, where topics include advances in the visualization and identification of photo-reaction dynamics of biological functions under relevant physiological conditions, theoretically proposed imaging designs for obtaining super-resolved optical sectioned images in single exposures and fabricated micro-structured surfaces for biological micro-environments. We hope the collection will stimulate innovative new research in this growing field by showcasing new techniques for the visualization and manipulation of complex biological systems using linear and and nonlinear optical processes. Professor Min Gu would like to acknowledge Dr Betty Kouskousis for her contribution and support towards this editorial.

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

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

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

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

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

DOE PAGES

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

2016-12-27

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

X-ray phase contrast imaging of biological specimens with femtosecond pulses of betatron radiation from a compact laser plasma wakefield accelerator

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

Kneip, S.; Center for Ultrafast Optical Science, University of Michigan, Ann Arbor 48109; McGuffey, C.

2011-08-29

We show that x-rays from a recently demonstrated table top source of bright, ultrafast, coherent synchrotron radiation [Kneip et al., Nat. Phys. 6, 980 (2010)] can be applied to phase contrast imaging of biological specimens. Our scheme is based on focusing a high power short pulse laser in a tenuous gas jet, setting up a plasma wakefield accelerator that accelerates and wiggles electrons analogously to a conventional synchrotron, but on the centimeter rather than tens of meter scale. We use the scheme to record absorption and phase contrast images of a tetra fish, damselfly and yellow jacket, in particular highlightingmore » the contrast enhancement achievable with the simple propagation technique of phase contrast imaging. Coherence and ultrafast pulse duration will allow for the study of various aspects of biomechanics.« less

Nonequilibrium dynamics of the phonon gas in ultrafast-excited antimony

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Diffuse shear wave imaging: toward passive elastography using low-frame rate spectral-domain optical coherence tomography

NASA Astrophysics Data System (ADS)

Nguyen, Thu-Mai; Zorgani, Ali; Lescanne, Maxime; Boccara, Claude; Fink, Mathias; Catheline, Stefan

2016-12-01

Optical coherence tomography (OCT) can map the stiffness of biological tissue by imaging mechanical perturbations (shear waves) propagating in the tissue. Most shear wave elastography (SWE) techniques rely on active shear sources to generate controlled displacements that are tracked at ultrafast imaging rates. Here, we propose a noise-correlation approach to retrieve stiffness information from the imaging of diffuse displacement fields using low-frame rate spectral-domain OCT. We demonstrated the method on tissue-mimicking phantoms and validated the results by comparison with classic ultrafast SWE. Then we investigated the in vivo feasibility on the eye of an anesthetized rat by applying noise correlation to naturally occurring displacements. The results suggest a great potential for passive elastography based on the detection of natural pulsatile motions using conventional spectral-domain OCT systems. This would facilitate the transfer of OCT-elastography to clinical practice, in particular, in ophthalmology or dermatology.

Diffuse shear wave imaging: toward passive elastography using low-frame rate spectral-domain optical coherence tomography.

PubMed

Nguyen, Thu-Mai; Zorgani, Ali; Lescanne, Maxime; Boccara, Claude; Fink, Mathias; Catheline, Stefan

2016-12-01

Optical coherence tomography (OCT) can map the stiffness of biological tissue by imaging mechanical perturbations (shear waves) propagating in the tissue. Most shear wave elastography (SWE) techniques rely on active shear sources to generate controlled displacements that are tracked at ultrafast imaging rates. Here, we propose a noise-correlation approach to retrieve stiffness information from the imaging of diffuse displacement fields using low-frame rate spectral-domain OCT. We demonstrated the method on tissue-mimicking phantoms and validated the results by comparison with classic ultrafast SWE. Then we investigated the in vivo feasibility on the eye of an anesthetized rat by applying noise correlation to naturally occurring displacements. The results suggest a great potential for passive elastography based on the detection of natural pulsatile motions using conventional spectral-domain OCT systems. This would facilitate the transfer of OCT-elastography to clinical practice, in particular, in ophthalmology or dermatology.

Ultrafast dynamics of multi-exciton state coupled to coherent vibration in zinc chlorin aggregates for artificial photosynthesis.

PubMed

Shi, Tongchao; Liu, Zhengzheng; Miyatake, Tomohiro; Tamiaki, Hitoshi; Kobayashi, Takayoshi; Zhang, Zeyu; Du, Juan; Leng, Yuxin

2017-11-27

Ultrafast vibronic dynamics induced by the interaction of the Frenkel exciton with the coherent molecular vibrations in a layer-structured zinc chlorin aggregates prepared for artificial photosynthesis have been studied by 7.1 fs real-time vibrational spectroscopy with multi-spectrum detection. The fast decay of 100 ± 5fs is ascribed to the relaxation from the higher multi-exciton state (MES) to the one-exciton state, and the slow one of 863 ± 70fs is assigned to the relaxation from Q-exciton state to the dark nonfluorescent charge-transfer (CT) state, respectively. In addition, the wavelength dependences of the exciton-vibration coupling strength are found to follow the zeroth derivative of the transient absorption spectra of the exciton. It could be explained in term of the transition dipole moment modulated by dynamic intensity borrowing between the B transition and the Q transition through the vibronic interactions.

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

NASA Astrophysics Data System (ADS)

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

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

Ultrafast 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.

Seeing with the nano-eye: accessing structure, function, and dynamics of matter on its natural length and time scales

NASA Astrophysics Data System (ADS)

Raschke, Markus

2015-03-01

To understand and ultimately control the properties of most functional materials, from molecular soft-matter to quantum materials, requires access to the structure, coupling, and dynamics on the elementary time and length scales that define the microscopic interactions in these materials. To gain the desired nanometer spatial resolution with simultaneous spectroscopic specificity we combine scanning probe microscopy with different optical, including coherent, nonlinear, and ultrafast spectroscopies. The underlying near-field interaction mediated by the atomic-force or scanning tunneling microscope tip provides the desired deep-sub wavelength nano-focusing enabling few-nm spatial resolution. I will introduce our generalization of the approach in terms of the near-field impedance matching to a quantum system based on special optical antenna-tip designs. The resulting enhanced and qualitatively new forms of light-matter interaction enable measurements of quantum dynamics in an interacting environment or to image the electromagnetic local density of states of thermal radiation. Other applications include the inter-molecular coupling and dynamics in soft-matter hetero-structures, surface plasmon interferometry as a probe of electronic structure and dynamics in graphene, and quantum phase transitions in correlated electron materials. These examples highlight the general applicability of the new near-field microscopy approach, complementing emergent X-ray and electron imaging tools, aiming towards the ultimate goal of probing matter on its most elementary spatio-temporal level.

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

PubMed

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

2013-03-01

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

Signal-to-noise ratios in coherent soft limiters

NASA Technical Reports Server (NTRS)

Lesh, J. R.

1973-01-01

Expressions for the output signal-to-noise power ratio of a bandpass soft limiter followed by a coherent detection device are presented and discussed. It is found that a significant improvement in the output signal-to-noise ratio at low input SNRs can be achieved by such soft limiters as compared to hard limiters. This indicates that the soft limiter may be of some use in the area of threshold extension. Approximation methods for determining output signal-to-noise spectral densities are also presented.

Single-pulse coherent diffraction imaging using soft x-ray laser.

PubMed

Kang, Hyon Chol; Kim, Hyung Taek; Kim, Sang Soo; Kim, Chan; Yu, Tae Jun; Lee, Seong Ku; Kim, Chul Min; Kim, I Jong; Sung, Jae Hee; Janulewicz, Karol A; Lee, Jongmin; Noh, Do Young

2012-05-15

We report a coherent diffraction imaging (CDI) using a single 8 ps soft x-ray laser pulse at a wavelength of 13.9 nm. The soft x-ray pulse was generated by a laboratory-scale intense pumping laser providing coherent x-ray pulses up to the level of 10(11) photons/pulse. A spatial resolution below 194 nm was achieved with a single pulse, and it was shown that a resolution below 55 nm is feasible with improved detector capability. The single-pulse CDI might provide a way to investigate dynamics of nanoscale molecules or particles.

High flux table-top ultrafast soft X-ray source generated by high harmonic generation

NASA Astrophysics Data System (ADS)

Thiré, Nicolas; Schmidt, Bruno E.; Fourmeaux, Sylvain; Beaulieu, Samuel; Cardin, Vincent; Negro, Matteo; Kieffer, Jean-Claude; Vozzi, Caterina; Legare, François

2014-05-01

Generation of ultrafast soft X-ray pulses is a major challenge for conventional laboratories. Using the process of HHG enables generation of such short wavelength photons. Intense laser sources in the infrared are necessary to reach the soft X-ray spectral range as the HHG cut-off scales with Iλ2. However, in the limit of the single atom response, increasing the laser wavelength leads to a significant decrease of the HHG flux. To compensate, one has to increase the number of emitters with high ionization potential. At the Advanced Laser Light Source, we have addressed this challenge by using a new gas cell design and developing a 10 mJ - 30 fs source at 1.8 μm. Using this setup, we have been able to generate harmonics in the water window spectral range for neon and helium with short time duration (<30 fs) in a conventional laboratory. A flux measurement has been performed showing ~ 2 × 105 photons/shot between 280 and 540 eV, making it possible to see the carbon k-edge at 280eV in a single shot manner. This soft X-ray beam is also extremely well collimated (0.1 mrad) making it this table-top beamline ideal for a number of applications.

Ultrafast Pulse Generation in an Organic Nanoparticle-Array Laser.

PubMed

Daskalakis, Konstantinos S; Väkeväinen, Aaro I; Martikainen, Jani-Petri; Hakala, Tommi K; Törmä, Päivi

2018-04-11

Nanoscale coherent light sources offer potentially ultrafast modulation speeds, which could be utilized for novel sensors and optical switches. Plasmonic periodic structures combined with organic gain materials have emerged as promising candidates for such nanolasers. Their plasmonic component provides high intensity and ultrafast nanoscale-confined electric fields, while organic gain materials offer fabrication flexibility and a low acquisition cost. Despite reports on lasing in plasmonic arrays, lasing dynamics in these structures have not been experimentally studied yet. Here we demonstrate, for the first time, an organic dye nanoparticle-array laser with more than a 100 GHz modulation bandwidth. We show that the lasing modulation speed can be tuned by the array parameters. Accelerated dynamics is observed for plasmonic lasing modes at the blue side of the dye emission.

Time-dependent nonequilibrium soft x-ray response during a spin crossover

NASA Astrophysics Data System (ADS)

van Veenendaal, Michel

2018-03-01

A theoretical framework is developed for better understanding the time-dependent soft-x-ray response of dissipative quantum many-body systems. It is shown how x-ray absorption and resonant inelastic x-ray scattering (RIXS) at transition-metal L edges can provide insight into ultrafast intersystem crossings of importance for energy conversion, ultrafast magnetism, and catalysis. The photoinduced doublet-to-quartet spin crossover on cobalt in Fe-Co Prussian blue analogs is used as a model system to demonstrate how the x-ray response is affected by the nonequilibrium dynamics on a femtosecond time scale. Changes in local spin and symmetry and the underlying mechanism are reflected in strong broadenings, a collapse of clear selection rules during the intersystem crossing, fluctuations in the isotropic branching ratio in x-ray absorption, crystal-field collapse and/or oscillations, and time-dependent anti-Stokes processes in RIXS.

Quantum coherent π-electron rotations in a non-planar chiral molecule induced by using a linearly polarized UV laser pulse

NASA Astrophysics Data System (ADS)

Mineo, Hirobumi; Fujimura, Yuichi

2015-06-01

We propose an ultrafast quantum switching method of π-electron rotations, which are switched among four rotational patterns in a nonplanar chiral aromatic molecule (P)-2,2’- biphenol and perform the sequential switching among four rotational patterns which are performed by the overlapped pump-dump laser pulses. Coherent π-electron dynamics are generated by applying the linearly polarized UV pulse laser to create a pair of coherent quasidegenerated excited states. We also plot the time-dependent π-electron ring current, and discussed ring current transfer between two aromatic rings.

Ultrafast Coherent Dynamics of a Photonic Crystal All-Optical Switch.

PubMed

Colman, Pierre; Lunnemann, Per; Yu, Yi; Mørk, Jesper

2016-12-02

We present pump-probe measurements of an all-optical photonic crystal switch based on a nanocavity, resolving fast coherent temporal dynamics. The measurements demonstrate the importance of coherent effects typically neglected when considering nanocavity dynamics. In particular, we report the observation of an idler pulse and more than 10 dB parametric gain. The measurements are in good agreement with a theoretical model that ascribes the observation to oscillations of the free-carrier population in the nanocavity. The effect opens perspectives for the realization of new all-optical photonic crystal switches with unprecedented switching contrast.

Effects of Different Quantum Coherence on the Pump-Probe Polarization Anisotropy of Photosynthetic Light-Harvesting Complexes: A Computational Study.

PubMed

Bai, Shuming; Song, Kai; Shi, Qiang

2015-05-21

Observations of oscillatory features in the 2D spectra of several photosynthetic complexes have led to diverged opinions on their origins, including electronic coherence, vibrational coherence, and vibronic coherence. In this work, effects of these different types of quantum coherence on ultrafast pump-probe polarization anisotropy are investigated and distinguished. We first simulate the isotropic pump-probe signal and anisotropy decay of the Fenna-Matthews-Olson (FMO) complex using a model with only electronic coherence at low temperature and obtain the same coherence time as in the previous experiment. Then, three model dimer systems with different prespecified quantum coherence are simulated, and the results show that their different spectral characteristics can be used to determine the type of coherence during the spectral process. Finally, we simulate model systems with different electronic-vibrational couplings and reveal the condition in which long time vibronic coherence can be observed in systems like the FMO complex.

Ultrafast X-Ray Coherent Control

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

Reis, David

2009-05-01

This main purpose of this grant was to develop the nascent eld of ultrafast x-ray science using accelerator-based sources, and originally developed from an idea that a laser could modulate the di racting properties of a x-ray di racting crystal on a fast enough time scale to switch out in time a shorter slice from the already short x-ray pulses from a synchrotron. The research was carried out primarily at the Advanced Photon Source (APS) sector 7 at Argonne National Laboratory and the Sub-Picosecond Pulse Source (SPPS) at SLAC; in anticipation of the Linac Coherent Light Source (LCLS) x-ray freemore » electron laser that became operational in 2009 at SLAC (all National User Facilities operated by BES). The research centered on the generation, control and measurement of atomic-scale dynamics in atomic, molecular optical and condensed matter systems with temporal and spatial resolution . It helped develop the ultrafast physics, techniques and scienti c case for using the unprecedented characteristics of the LCLS. The project has been very successful with results have been disseminated widely and in top journals, have been well cited in the eld, and have laid the foundation for many experiments being performed on the LCLS, the world's rst hard x-ray free electron laser.« less

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

NASA Astrophysics Data System (ADS)

Gulliford, Colwyn; Bartnik, Adam; Bazarov, Ivan

2016-09-01

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

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

NASA Astrophysics Data System (ADS)

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

2013-12-01

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

Picosecond phase-velocity dispersion of hypersonic phonons imaged with ultrafast electron microscopy

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

Cremons, Daniel R.; Du, Daniel X.; Flannigan, David J.

We describe the direct imaging—with four-dimensional ultrafast electron microscopy—of the emergence, evolution, dispersion, and decay of photoexcited, hypersonic coherent acoustic phonons in nanoscale germanium wedges. Coherent strain waves generated via ultrafast in situ photoexcitation were imaged propagating with initial phase velocities of up to 35 km/s across discrete micrometer-scale crystal regions. We then observe that, while each wave front travels at a constant velocity, the entire wave train evolves with a time-varying phase-velocity dispersion, displaying a single-exponential decay to the longitudinal speed of sound (5 km/s) and with a mean lifetime of 280 ps. We also find that the wavemore » trains propagate along a single in-plane direction oriented parallel to striations introduced during specimen preparation, independent of crystallographic direction. Elastic-plate modeling indicates the dynamics arise from excitation of a single, symmetric (dilatational) guided acoustic mode. Further, by precisely determining the experiment time-zero position with a plasma-lensing method, we find that wave-front emergence occurs approximately 100 ps after femtosecond photoexcitation, which matches well with Auger recombination times in germanium. We conclude by discussing the similarities between the imaged hypersonic strain-wave dynamics and electron/hole plasma-wave dynamics in strongly photoexcited semiconductors.« less

Picosecond phase-velocity dispersion of hypersonic phonons imaged with ultrafast electron microscopy

DOE PAGES

Cremons, Daniel R.; Du, Daniel X.; Flannigan, David J.

2017-12-05

We describe the direct imaging—with four-dimensional ultrafast electron microscopy—of the emergence, evolution, dispersion, and decay of photoexcited, hypersonic coherent acoustic phonons in nanoscale germanium wedges. Coherent strain waves generated via ultrafast in situ photoexcitation were imaged propagating with initial phase velocities of up to 35 km/s across discrete micrometer-scale crystal regions. We then observe that, while each wave front travels at a constant velocity, the entire wave train evolves with a time-varying phase-velocity dispersion, displaying a single-exponential decay to the longitudinal speed of sound (5 km/s) and with a mean lifetime of 280 ps. We also find that the wavemore » trains propagate along a single in-plane direction oriented parallel to striations introduced during specimen preparation, independent of crystallographic direction. Elastic-plate modeling indicates the dynamics arise from excitation of a single, symmetric (dilatational) guided acoustic mode. Further, by precisely determining the experiment time-zero position with a plasma-lensing method, we find that wave-front emergence occurs approximately 100 ps after femtosecond photoexcitation, which matches well with Auger recombination times in germanium. We conclude by discussing the similarities between the imaged hypersonic strain-wave dynamics and electron/hole plasma-wave dynamics in strongly photoexcited semiconductors.« less

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

PubMed

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

2017-10-18

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

Ultrafast X-ray diffraction probe of terahertz field-driven soft mode dynamics in SrTiO 3

DOE PAGES

Kozina, M.; van Driel, T.; Chollet, M.; ...

2017-05-03

We use ultrafast x-ray pulses to characterize the lattice response of SrTiO 3 when driven by strong terahertz (THz) fields. We observe transient changes in the diffraction intensity with a delayed onset with respect to the driving field. Fourier analysis reveals two frequency components corresponding to the two lowest energy zone-center optical modes in SrTiO 3. Lastly, the lower frequency mode exhibits clear softening as the temperature is decreased while the higher frequency mode shows slight temperature dependence.

Ultrafast Independent N-H and N-C Bond Deformation Investigated with Resonant Inelastic X-Ray Scattering

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

Eckert, Sebastian; Norell, Jesper; Miedema, Piter S.

Here, the femtosecond excited-state dynamics following resonant photoexcitation enable the selective deformation of N-H and N-C chemical bonds in 2-thiopyridone in aqueous solution with optical or X-ray pulses. In combination with multiconfigurational quantum-chemical calculations, the orbital-specific electronic structure and its ultrafast dynamics accessed with resonant inelastic X-ray scattering at the N 1s level using synchrotron radiation and the soft X-ray free-electron laser LCLS provide direct evidence for this controlled photoinduced molecular deformation and its ultrashort timescale.

Ultrafast Independent N-H and N-C Bond Deformation Investigated with Resonant Inelastic X-Ray Scattering

DOE PAGES

Eckert, Sebastian; Norell, Jesper; Miedema, Piter S.; ...

2017-04-04

Here, the femtosecond excited-state dynamics following resonant photoexcitation enable the selective deformation of N-H and N-C chemical bonds in 2-thiopyridone in aqueous solution with optical or X-ray pulses. In combination with multiconfigurational quantum-chemical calculations, the orbital-specific electronic structure and its ultrafast dynamics accessed with resonant inelastic X-ray scattering at the N 1s level using synchrotron radiation and the soft X-ray free-electron laser LCLS provide direct evidence for this controlled photoinduced molecular deformation and its ultrashort timescale.

Ultrafast X-ray diffraction probe of terahertz field-driven soft mode dynamics in SrTiO 3

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

Kozina, M.; van Driel, T.; Chollet, M.

We use ultrafast x-ray pulses to characterize the lattice response of SrTiO 3 when driven by strong terahertz (THz) fields. We observe transient changes in the diffraction intensity with a delayed onset with respect to the driving field. Fourier analysis reveals two frequency components corresponding to the two lowest energy zone-center optical modes in SrTiO 3. Lastly, the lower frequency mode exhibits clear softening as the temperature is decreased while the higher frequency mode shows slight temperature dependence.

Ultrafast Exciton Delocalization, Localization, and Excimer Formation Dynamics in a Highly Defined Perylene Bisimide Quadruple π-Stack.

PubMed

Kaufmann, Christina; Kim, Woojae; Nowak-Król, Agnieszka; Hong, Yongseok; Kim, Dongho; Würthner, Frank

2018-03-28

An adequately designed, bay-tethered perylene bisimide (PBI) dimer Bis-PBI was synthesized by Pd/Cu-catalyzed Glaser-type oxidative homocoupling of the respective PBI building block. This newly synthesized PBI dimer self-assembles exclusively and with high binding constants of up to 10 6 M -1 into a discrete π-stack of four chromophores. Steady-state absorption and emission spectra show the signatures of H-type excitonic coupling among the dye units. Broadband fluorescence upconversion spectroscopy (FLUPS) reveals an ultrafast dynamics in the optically excited state. An initially coherent Frenkel exciton state that is delocalized over the whole quadruple stack rapidly (τ = ∼200 fs) loses its coherence and relaxes into an excimer state. Comparison with Frenkel exciton dynamics in PBI dimeric and oligomeric H-aggregates demonstrates that in the quadruple stack coherent exciton propagation is absent due to its short length of aggregates, thereby it has only one relaxation pathway to the excimer state. Furthermore, the absence of pump-power dependence in transient absorption experiments suggests that multiexciton cannot be generated in the quadruple stack, which is in line with time-resolved fluorescence measurements.

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.

Hot spot-mediated non-dissipative and ultrafast plasmon passage.

PubMed

Roller, Eva-Maria; Besteiro, Lucas V; Pupp, Claudia; Khorashad, Larousse Khosravi; Govorov, Alexander O; Liedl, Tim

2017-08-01

Plasmonic nanoparticles hold great promise as photon handling elements and as channels for coherent transfer of energy and information in future all-optical computing devices.1-5 Coherent energy oscillations between two spatially separated plasmonic entities via a virtual middle state exemplify electron-based population transfer, but their realization requires precise nanoscale positioning of heterogeneous particles.6-10 Here, we show the assembly and optical analysis of a triple particle system consisting of two gold nanoparticles with an inter-spaced silver island. We observe strong plasmonic coupling between the spatially separated gold particles mediated by the connecting silver particle with almost no dissipation of energy. As the excitation energy of the silver island exceeds that of the gold particles, only quasi-occupation of the silver transfer channel is possible. We describe this effect both with exact classical electrodynamic modeling and qualitative quantum-mechanical calculations. We identify the formation of strong hot spots between all particles as the main mechanism for the loss-less coupling and thus coherent ultra-fast energy transfer between the remote partners. Our findings could prove useful for quantum gate operations, but also for classical charge and information transfer processes.

Solution Phase Exciton Diffusion Dynamics of a Charge-Transfer Copolymer PTB7 and a Homopolymer P3HT

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

Cho, Sung; Rolczynski, Brian S.; Xu, Tao

2015-06-18

Using ultrafast polarization-controlled transient absorption (TA) measurements, dynamics of the initial exciton states were investigated on the time scale of tens of femtoseconds to about 80 ps in two different types of conjugated polymers extensively used in active layers of organic photovoltaic devices. These polymers are poly(3-fluorothienothiophenebenzodithiophene) (PTB7) and poly-3-hexylthiophene (P3HT), which are charge-transfer polymers and homopolymers, respectively. In PTB7, the initial excitons with excess vibrational energy display two observable ultrafast time constants, corresponding to coherent exciton diffusion before the vibrational relaxation, and followed by incoherent exciton diffusion processes to a neighboring local state after the vibrational relaxation. In contrast,more » P3HT shows only one exciton diffusion or conformational motion time constant of 34 ps, even though its exciton decay kinetics are multiexponential. Based on the experimental results, an exciton dynamics mechanism is conceived taking into account the excitation energy and structural dependence in coherent and incoherent exciton diffusion processes, as well as other possible deactivation processes including the formation of the pseudo-charge-transfer and charge separate states, as well as interchain exciton hopping or coherent diffusion.« less

Solution Phase Exciton Diffusion Dynamics of a Charge-Transfer Copolymer PTB7 and a Homopolymer P3HT.

PubMed

Cho, Sung; Rolczynski, Brian S; Xu, Tao; Yu, Luping; Chen, Lin X

2015-06-18

Using ultrafast polarization-controlled transient absorption (TA) measurements, dynamics of the initial exciton states were investigated on the time scale of tens of femtoseconds to about 80 ps in two different types of conjugated polymers extensively used in active layers of organic photovoltaic devices. These polymers are poly(3-fluorothienothiophenebenzodithiophene) (PTB7) and poly-3-hexylthiophene (P3HT), which are charge-transfer polymers and homopolymers, respectively. In PTB7, the initial excitons with excess vibrational energy display two observable ultrafast time constants, corresponding to coherent exciton diffusion before the vibrational relaxation, and followed by incoherent exciton diffusion processes to a neighboring local state after the vibrational relaxation. In contrast, P3HT shows only one exciton diffusion or conformational motion time constant of 34 ps, even though its exciton decay kinetics are multiexponential. Based on the experimental results, an exciton dynamics mechanism is conceived taking into account the excitation energy and structural dependence in coherent and incoherent exciton diffusion processes, as well as other possible deactivation processes including the formation of the pseudo-charge-transfer and charge separate states, as well as interchain exciton hopping or coherent diffusion.

Coherent Excitation of Optical Phonons in GaAs by Broadband Terahertz Pulses

PubMed Central

Fu, Zhengping; Yamaguchi, Masashi

2016-01-01

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

Possible Demonstration of a Polaronic Bose-Einstein(-Mott) Condensate in UO 2(+x) by Ultrafast THz Spectroscopy and Microwave Dissipation

DOE PAGES

Conradson, Steven D.; Gilbertson, Steven M.; Daifuku, Stephanie L.; ...

2015-10-16

Bose-Einstein condensates (BECs) composed of polarons would be an advance because they would combine coherently charge, spin, and a crystal lattice. Following our earlier report of unique structural and spectroscopic properties, we now identify potentially definitive evidence for polaronic BECs in photo- and chemically doped UO 2(+x) on the basis of exceptional coherence in the ultrafast time dependent terahertz absorption and microwave spectroscopy results that show collective behavior including dissipation patterns whose precedents are condensate vortex and defect disorder and condensate excitations. Furthermore, that some of these signatures of coherence in an atom-based system extend to ambient temperature suggests amore » novel mechanism that could be a synchronized, dynamical, disproportionation excitation, possibly via the solid state analog of a Feshbach resonance that promotes the coherence. Such a mechanism would demonstrate that the use of ultra-low temperatures to establish the BEC energy distribution is a convenience rather than a necessity, with the actual requirement for the particles being in the same state that is not necessarily the ground state attainable by other means. Interestingly, a macroscopic quantum object created by chemical doping that can persist to ambient temperature and resides in a bulk solid would be revolutionary in a number of scientific and technological fields.« less

Possible Demonstration of a Polaronic Bose-Einstein(-Mott) Condensate in UO 2(+x) by Ultrafast THz Spectroscopy and Microwave Dissipation

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

Conradson, Steven D.; Gilbertson, Steven M.; Daifuku, Stephanie L.

Bose-Einstein condensates (BECs) composed of polarons would be an advance because they would combine coherently charge, spin, and a crystal lattice. Following our earlier report of unique structural and spectroscopic properties, we now identify potentially definitive evidence for polaronic BECs in photo- and chemically doped UO 2(+x) on the basis of exceptional coherence in the ultrafast time dependent terahertz absorption and microwave spectroscopy results that show collective behavior including dissipation patterns whose precedents are condensate vortex and defect disorder and condensate excitations. Furthermore, that some of these signatures of coherence in an atom-based system extend to ambient temperature suggests amore » novel mechanism that could be a synchronized, dynamical, disproportionation excitation, possibly via the solid state analog of a Feshbach resonance that promotes the coherence. Such a mechanism would demonstrate that the use of ultra-low temperatures to establish the BEC energy distribution is a convenience rather than a necessity, with the actual requirement for the particles being in the same state that is not necessarily the ground state attainable by other means. Interestingly, a macroscopic quantum object created by chemical doping that can persist to ambient temperature and resides in a bulk solid would be revolutionary in a number of scientific and technological fields.« less

Single-particle coherent diffractive imaging with a soft x-ray free electron laser: towards soot aerosol morphology

NASA Astrophysics Data System (ADS)

Bogan, Michael J.; Starodub, Dmitri; Hampton, Christina Y.; Sierra, Raymond G.

2010-10-01

The first of its kind, the Free electron LASer facility in Hamburg, FLASH, produces soft x-ray pulses with unprecedented properties (10 fs, 6.8-47 nm, 1012 photons per pulse, 20 µm diameter). One of the seminal FLASH experiments is single-pulse coherent x-ray diffractive imaging (CXDI). CXDI utilizes the ultrafast and ultrabright pulses to overcome resolution limitations in x-ray microscopy imposed by x-ray-induced damage to the sample by 'diffracting before destroying' the sample on sub-picosecond timescales. For many lensless imaging algorithms used for CXDI it is convenient when the data satisfy an oversampling constraint that requires the sample to be an isolated object, i.e. an individual 'free-standing' portion of disordered matter delivered to the centre of the x-ray focus. By definition, this type of matter is an aerosol. This paper will describe the role of aerosol science methodologies used for the validation of the 'diffract before destroy' hypothesis and the execution of the first single-particle CXDI experiments being developed for biological imaging. FLASH CXDI now enables the highest resolution imaging of single micron-sized or smaller airborne particulate matter to date while preserving the native substrate-free state of the aerosol. Electron microscopy offers higher resolution for single-particle analysis but the aerosol must be captured on a substrate, potentially modifying the particle morphology. Thus, FLASH is poised to contribute significant advancements in our knowledge of aerosol morphology and dynamics. As an example, we simulate CXDI of combustion particle (soot) morphology and introduce the concept of extracting radius of gyration of fractal aggregates from single-pulse x-ray diffraction data. Future upgrades to FLASH will enable higher spatially and temporally resolved single-particle aerosol dynamics studies, filling a critical technological need in aerosol science and nanotechnology. Many of the methodologies described for FLASH will directly translate to use at hard x-ray free electron lasers.

Reversible ultrafast melting in bulk CdSe

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

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

2016-02-07

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

Ultrafast electric phase control of a single exciton qubit

NASA Astrophysics Data System (ADS)

Widhalm, Alex; Mukherjee, Amlan; Krehs, Sebastian; Sharma, Nandlal; Kölling, Peter; Thiede, Andreas; Reuter, Dirk; Förstner, Jens; Zrenner, Artur

2018-03-01

We report on the coherent phase manipulation of quantum dot excitons by electric means. For our experiments, we use a low capacitance single quantum dot photodiode which is electrically controlled by a custom designed SiGe:C BiCMOS chip. The phase manipulation is performed and quantified in a Ramsey experiment, where ultrafast transient detuning of the exciton energy is performed synchronous to double pulse π/2 ps laser excitation. We are able to demonstrate electrically controlled phase manipulations with magnitudes up to 3π within 100 ps which is below the dephasing time of the quantum dot exciton.

Model of THz Magnetization Dynamics.

PubMed

Bocklage, Lars

2016-03-09

Magnetization dynamics can be coherently controlled by THz laser excitation, which can be applied in ultrafast magnetization control and switching. Here, transient magnetization dynamics are calculated for excitation with THz magnetic field pulses. We use the ansatz of Smit and Beljers, to formulate dynamic properties of the magnetization via partial derivatives of the samples free energy density, and extend it to solve the Landau-Lifshitz-equation to obtain the THz transients of the magnetization. The model is used to determine the magnetization response to ultrafast multi- and single-cycle THz pulses. Control of the magnetization trajectory by utilizing the THz pulse shape and polarization is demonstrated.

Time resolved 3D momentum imaging of ultrafast dynamics by coherent VUV-XUV radiation

DOE PAGES

Sturm, F. P.; Wright, T. W.; Ray, D.; ...

2016-06-14

Have we present a new experimental setup for measuring ultrafast nuclear and electron dynamics of molecules after photo-excitation and ionization. We combine a high flux femtosecond vacuum ultraviolet (VUV) and extreme ultraviolet (XUV) source with an internally cold molecular beam and a 3D momentum imaging particle spectrometer to measure electrons and ions in coincidence. We describe a variety of tools developed to perform pump-probe studies in the VUV-XUV spectrum and to modify and characterize the photon beam. First benchmark experiments are presented to demonstrate the capabilities of the system.

Coherent Femtosecond Spectroscopy and Nonlinear Optical Imaging on the Nanoscale

NASA Astrophysics Data System (ADS)

Kravtsov, Vasily

Optical properties of many materials and macroscopic systems are defined by ultrafast dynamics of electronic, vibrational, and spin excitations localized on the nanoscale. Harnessing these excitations for material engineering, optical computing, and control of chemical reactions has been a long-standing goal in science and technology. However, it is challenging due to the lack of spectroscopic techniques that can resolve processes simultaneously on the nanometer spatial and femtosecond temporal scales. This thesis describes the fundamental principles, implementation, and experimental demonstration of a novel type of ultrafast microscopy based on the concept of adiabatic plasmonic nanofocusing. Simultaneous spatio-temporal resolution on a nanometer-femtosecond scale is achieved by using a near-field nonlinear optical response induced by ultrafast surface plasmon polaritons nanofocused on a metal tip. First, we study the surface plasmon response in metallic structures and evaluate its prospects and limitations for ultrafast near-field microscopy. Through plasmon emission-based spectroscopy, we investigate dephasing times and interplay between radiative and non-radiative decay rates of localized plasmons and their modification due to coupling. We identify a new regime of quantum plasmonic coupling, which limits the achievable spatial resolution to several angstroms but at the same time provides a potential channel for generating ultrafast electron currents at optical frequencies. Next, we study propagation of femtosecond wavepackets of surface plasmon polaritons on a metal tip. In time-domain interferometric measurements we detect group delays that correspond to slowing of the plasmon polaritons down to 20% of the speed of light at the tip apex. This provides direct experimental verification of the plasmonic nanofocusing mechanism and suggests enhanced nonlinear optical interactions at the tip apex. We then measure a plasmon-generated third-order nonlinear optical four-wave mixing response from the tip apex and investigate its microscopic mechanism. Our results reveal a significant contribution to the third order nonlinearity of plasmonic structures due to large near-field gradients associated with nanofocused plasmons. In combination with scanning probe imaging and femtosecond pulse shaping, the nanofocused four-wave mixing response provides a basis for a novel type of ultrafast optical microscopy on the nanoscale. We demonstrate its capabilities by nano-imaging the coherent dynamics of localized plasmonic modes in a rough gold film edge with simultaneous sub-50 nm spatial and sub-5 fs temporal resolution. We capture the coherent decay and extract the dephasing times of individual plasmonic modes. Lastly, we apply our technique to study nanoscale spatial heterogeneity of the nonlinear optical response in novel two-dimensional materials: monolayer and few-layer graphene. An enhanced four-wave mixing signal is revealed on the edges of graphene flakes. We investigate the mechanism of this enhancement by performing nano-imaging on a graphene field-effect transistor with the variable carrier density controlled by electrostatic gating.

Semiclassical study of quantum coherence and isotope effects in ultrafast electron transfer reactions coupled to a proton and a phonon bath.

PubMed

Venkataraman, Charulatha

2011-11-28

The linearized semiclassical initial value representation is employed to describe ultrafast electron transfer processes coupled to a phonon bath and weakly coupled to a proton mode. The goal of our theoretical investigation is to understand the influence of the proton on the electronic dynamics in various bath relaxation regimes. More specifically, we study the impact of the proton on coherences and analyze if the coupling to the proton is revealed in the form of an isotope effect. This will be important in distinguishing reactions in which the proton does not undergo significant rearrangement from those in which the electron transfer is accompanied by proton transfer. Unlike other methodologies widely employed to describe nonadiabatic electron transfer, this approach treats the electronic and nuclear degrees of freedom consistently. However, due to the linearized approximation, quantum interference effects are not captured accurately. Our study shows that at small phonon bath reorganization energies, coherent oscillations and isotope effect are observed in both slow and fast bath regimes. The coherences are more substantially damped by deuterium in comparison to the proton. Further, in contrast to the dynamics of the spin-boson model, the coherences are not long-lived. At large bath reorganization energies, the decay is incoherent in the slow and fast bath regimes. In this case, the extent of the isotope effect depends on the relative relaxation timescales of the proton mode and the phonon bath. The isotope effect is magnified for baths that relax on picosecond timescales in contrast to baths that relax in femtoseconds.

Spin-analyzed SANS for soft matter applications

NASA Astrophysics Data System (ADS)

Chen, W. C.; Barker, J. G.; Jones, R.; Krycka, K. L.; Watson, S. M.; Gagnon, C.; Perevozchivoka, T.; Butler, P.; Gentile, T. R.

2017-06-01

The small angle neutron scattering (SANS) of nearly Q-independent nuclear spin-incoherent scattering from hydrogen present in most soft matter and biology samples may raise an issue in structure determination in certain soft matter applications. This is true at high wave vector transfer Q where coherent scattering is much weaker than the nearly Q-independent spin-incoherent scattering background. Polarization analysis is capable of separating coherent scattering from spin-incoherent scattering, hence potentially removing the nearly Q-independent background. Here we demonstrate SANS polarization analysis in conjunction with the time-of-flight technique for separation of coherent and nuclear spin-incoherent scattering for a sample of silver behenate back-filled with light water. We describe a complete procedure for SANS polarization analysis for separating coherent from incoherent scattering for soft matter samples that show inelastic scattering. Polarization efficiency correction and subsequent separation of the coherent and incoherent scattering have been done with and without a time-of-flight technique for direct comparisons. In addition, we have accounted for the effect of multiple scattering from light water to determine the contribution of nuclear spin-incoherent scattering in both the spin flip channel and non-spin flip channel when performing SANS polarization analysis. We discuss the possible gain in the signal-to-noise ratio for the measured coherent scattering signal using polarization analysis with the time-of-flight technique compared with routine unpolarized SANS measurements.

Coherent Raman Studies of Shocked Liquids

NASA Astrophysics Data System (ADS)

McGrane, Shawn; Brown, Kathryn; Dang, Nhan; Bolme, Cynthia; Moore, David

2013-06-01

Transient vibrational spectroscopies offer the potential to directly observe time dependent shock induced chemical reaction kinetics. We report recent experiments that couple a hybrid picosecond/femtosecond coherent anti-Stokes Raman spectroscopy (CARS) diagnostic with our tabletop ultrafast laser driven shock platform. Initial results on liquids shocked to 20 GPa suggest that sub-picosecond dephasing at high pressure and temperature may limit the application of this nonresonant background free version of CARS. Initial results using interferometric CARS to increase sensitivity and overcome these limitations will be presented.

A versatile setup for ultrafast broadband optical spectroscopy of coherent collective modes in strongly correlated quantum systems

PubMed Central

Baldini, Edoardo; Mann, Andreas; Borroni, Simone; Arrell, Christopher; van Mourik, Frank; Carbone, Fabrizio

2016-01-01

A femtosecond pump-probe setup is described that is optimised for broadband transient reflectivity experiments on solid samples over a wide temperature range. By combining high temporal resolution and a broad detection window, this apparatus can investigate the interplay between coherent collective modes and high-energy electronic excitations, which is a distinctive characteristic of correlated electron systems. Using a single-shot readout array detector at frame rates of 10 kHz allows resolving coherent oscillations with amplitudes <10−4. We demonstrate its operation on the charge-transfer insulator La2CuO4, revealing coherent phonons with frequencies up to 13 THz and providing access into their Raman matrix elements. PMID:27990455

Dynamics of plasmonic field polarization induced by quantum coherence in quantum dot-metallic nanoshell structures.

PubMed

Sadeghi, S M

2014-09-01

When a hybrid system consisting of a semiconductor quantum dot and a metallic nanoparticle interacts with a laser field, the plasmonic field of the metallic nanoparticle can be normalized by the quantum coherence generated in the quantum dot. In this Letter, we study the states of polarization of such a coherent-plasmonic field and demonstrate how these states can reveal unique aspects of the collective molecular properties of the hybrid system formed via coherent exciton-plasmon coupling. We show that transition between the molecular states of this system can lead to ultrafast polarization dynamics, including sudden reversal of the sense of variations of the plasmonic field and formation of circular and elliptical polarization.

Spectrally resolved femtosecond photon echo spectroscopy of astaxanthin

NASA Astrophysics Data System (ADS)

Kumar, Ajitesh; Karthick Kumar, S. K.; Gupta, Aditya; Goswami, Debabrata

2010-12-01

We have studied the coherence and population dynamics of Astaxanthin solution in methanol and acetonitrile by spectrally resolving their photon echo signals. Our experiments indicate that methanol has a much stronger interaction with the ultrafast dynamics of Astaxanthin in comparison to that of acetonitrile.

Spectrally resolved femtosecond photon echo spectroscopy of astaxanthin

NASA Astrophysics Data System (ADS)

Kumar, Ajitesh; Karthick Kumar, S. K.; Gupta, Aditya; Goswami, Debabrata

2011-08-01

We have studied the coherence and population dynamics of Astaxanthin solution in methanol and acetonitrile by spectrally resolving their photon echo signals. Our experiments indicate that methanol has a much stronger interaction with the ultrafast dynamics of Astaxanthin in comparison to that of acetonitrile.

Controlled ultrafast transfer and stability degree of generalized coherent states of a kicked two-level ion

NASA Astrophysics Data System (ADS)

Chen, Hao; Kong, Chao; Hai, Wenhua

2018-06-01

We investigate quantum dynamics of a two-level ion trapped in the Lamb-Dicke regime of a δ -kicked optical lattice, based on the exact generalized coherent states rotated by a π / 2 pulse of Ramsey type experiment. The spatiotemporal evolutions of the spin-motion entangled states in different parameter regions are illustrated, and the parameter regions of different degrees of quantum stability described by the quantum fidelity are found. Time evolutions of the probability for the ion being in different pseudospin states reveal that the ultrafast entanglement generation and population transfers of the system can be analytically controlled by managing the laser pulses. The probability in an initially disentangled state shows periodic collapses (entanglement) and revivals (de-entanglement). Reduction of the stability degree results in enlarging the period of de-entanglement, while the instability and potential chaos will cause the sustained entanglement. The results could be justified experimentally in the existing setups and may be useful in engineering quantum dynamics for quantum information processing.

Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells

PubMed Central

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

2016-01-01

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

Femtosecond two-photon Rabi oscillations in excited He driven by ultrashort intense laser fields

NASA Astrophysics Data System (ADS)

Fushitani, M.; Liu, C.-N.; Matsuda, A.; Endo, T.; Toida, Y.; Nagasono, M.; Togashi, T.; Yabashi, M.; Ishikawa, T.; Hikosaka, Y.; Morishita, T.; Hishikawa, A.

2016-02-01

Coherent light-matter interaction provides powerful methods for manipulating quantum systems. Rabi oscillation is one such process. As it enables complete population transfer to a target state, it is thus routinely exploited in a variety of applications in photonics, notably quantum information processing. The extension of coherent control techniques to the multiphoton regime offers wider applicability, and access to highly excited or dipole-forbidden transition states. However, the multiphoton Rabi process is often disrupted by other competing nonlinear effects such as the a.c. Stark shift, especially at the high laser-field intensities necessary to achieve ultrafast Rabi oscillations. Here we demonstrate a new route to drive two-photon Rabi oscillations on timescales as short as tens of femtoseconds, by utilizing the strong-field phenomenon known as Freeman resonance. The scenario is not specific to atomic helium as investigated in the present study, but broadly applicable to other systems, thus opening new prospects for the ultrafast manipulation of Rydberg states.

Ultrafast acousto-plasmonics in gold nanoparticle superlattices

NASA Astrophysics Data System (ADS)

Ruello, P.; Ayouch, A.; Vaudel, G.; Pezeril, T.; Delorme, N.; Sato, S.; Kimura, K.; Gusev, V. E.

2015-11-01

We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticle superlattices (NPSs). The experiments have been performed with an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow us to estimate first the fundamental mechanical parameters such as the collective elastic response (sound velocity) of the NPS and the nanocontact elastic stiffness. Furthermore, it appears that the light-induced coherent acoustic-phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly four times the optical skin depth in gold. The modeling of the transient optical reflectivity indicates that the mechanism of phonons generation is achieved through ultrafast heating of the NPS assisted by light excitation of the volume plasmon polariton. Based on these results, we demonstrate that it is possible to map the photon-electron-phonon interaction in subwavelength nanostructures which, in particular, provides insights on the fundamental properties of these nanometamaterials.

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.

Is back-electron transfer process in Betaine-30 coherent?

NASA Astrophysics Data System (ADS)

Rafiq, Shahnawaz; Scholes, Gregory D.

2017-09-01

The possible role of coherent vibrational motion in ultrafast photo-induced electron transfer remains unclear despite considerable experimental and theoretical advances. We revisited this problem by tracking the back-electron transfer (bET) process in Betaine-30 with broadband pump-probe spectroscopy. Dephasing time constant of certain high-frequency vibrations as a function of solvent shows a trend similar to the ET rates. In the purview of Bixon-Jortner model, high-frequency quantum vibrations bridge the reactant-product energy gap by providing activationless vibronic channels. Such interaction reduces the effective coupling significantly and thereby the coherence effects are eliminated due to energy gap fluctuations, making the back-electron transfer incoherent.

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.

Homepage P. Fischer, LBNL, Berkeley CA | UC Santa Cruz CA

Science.gov Websites

mesoscale magnetic x-ray microscopy and spectroscopy (ultra-)fast spin dynamics soft x-ray tomography of condensed matter x-ray optics publications presentations invited talks conference contributions curriculum

Invited Article: Coherent imaging using seeded free-electron laser pulses with variable polarization: First results and research opportunities

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

Capotondi, F.; Pedersoli, E.; Mahne, N.

2013-05-15

FERMI-Elettra, the first vacuum ultraviolet and soft X-ray free-electron laser (FEL) using by default a 'seeded' scheme, became operational in 2011 and has been opened to users since December 2012. The parameters of the seeded FERMI FEL pulses and, in particular, the superior control of emitted radiation in terms of spectral purity and stability meet the stringent requirements for single-shot and resonant coherent diffraction imaging (CDI) experiments. The advantages of the intense seeded FERMI pulses with variable polarization have been demonstrated with the first experiments performed using the multipurpose experimental station operated at the diffraction and projection imaging (DiProI) beamline.more » The results reported here were obtained with fixed non-periodic targets during the commissioning period in 2012 using 20-32 nm wavelength range. They demonstrate that the performance of the FERMI FEL source and the experimental station meets the requirements of CDI, holography, and resonant magnetic scattering in both multi- and single-shot modes. Moreover, we present the first magnetic scattering experiments employing the fully circularly polarized FERMI pulses. The ongoing developments aim at pushing the lateral resolution by using shorter wavelengths provided by double-stage cascaded FERMI FEL-2 and probing ultrafast dynamic processes using different pump-probe schemes, including jitter-free seed laser pump or FEL-pump/FEL-probe with two color FEL pulses generated by the same electron bunch.« less

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

Ultrafast studies of coexisting electronic order in cuprate superconductors

NASA Astrophysics Data System (ADS)

Hinton, James; Thewalt, Eric; Alpichshev, Zhanybek; Sternbach, Aaron; McLeod, Alex; Ji, L.; Veit, Mike; Dorrow, Chelsey; Koralek, Jake; Xhao, Xudong; Barisic, Neven; Kemper, Alexander; Gedik, Nuh; Greven, Martin; Basov, Dimitri; Orenstein, Joe

The cuprate family of high temperature superconductors displays a variety of electronic phases which emerge when charge carriers are added to the antiferromagnetic parent compound. These electronic phases are characterized by subtle differences in the low energy electronic excitations. Ultrafast time-resolved reflectivity (TRR) provides an ideal tool for investigating the cuprate phase diagram, as small changes in the electronic structure can produce significant contrast in the non-equilibrium reflectivity. Here we present TRR measurements of cuprate superconductors, focusing on the model single-layer cuprate HgBa2CuO4+δ. We observe a cusp-like feature in the quasiparticle lifetime near the superconducting transition temperature Tc. This feature can be understood using a model of coherently-mixed charge-density wave and superconducting pairing. We propose extending this technique to the nanoscale using ultrafast scattering scanning near-field microscopy (u-SNOM). This will allow us to explore how these electronic phases coexist and compete in real-space.

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

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

PubMed Central

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

2017-01-01

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

Single shot speckle and coherence analysis of the hard X-ray free electron laser LCLS

DOE PAGES

Lee, Sooheyong; Roseker, W.; Gutt, C.; ...

2013-10-08

The single shot based coherence properties of hard x-ray pulses from the Linac Coherent Light Source (LCLS) were measured by analyzing coherent diffraction patterns from nano-particles and gold nanopowder. The intensity histogram of the small angle x-ray scattering ring from nano-particles reveals the fully transversely coherent nature of the LCLS beam with a number of transverse modemore » $$\\langle$$M s$$\\rangle$$ = 1.1. On the other hand, the speckle contrasts measured at a large wavevector yields information about the longitudinal coherence of the LCLS radiation after a silicon (111) monochromator. The quantitative agreement between our data and the simulation confirms a mean coherence time of 2.2 fs and a x-ray pulse duration of 29 fs. Lastly the observed reduction of the speckle contrast generated by x-rays with pulse duration longer than 30 fs indicates ultrafast dynamics taking place at an atomic length scale prior to the permanent sample damage.« less

Nonlocal Electron Coherence in MoS2 Flakes Correlated through Spatial Self Phase Modulation

NASA Astrophysics Data System (ADS)

Wu, Yanling; Wu, Qiong; Sun, Fei; Tian, Yichao; Zuo, Xu; Meng, Sheng; Zhao, Jimin

2015-03-01

Electron coherence among different flake domains of MoS2 has been generated using ultrafast or continuous wave laser beams. Such electron coherence generates characteristic far-field diffraction patterns through a purely coherent nonlinear optical effect--spatial self-phase modulation (SSPM). A wind-chime model is developed to describe the establishment of the electron coherence through correlating the photo-excited electrons among different flakes using coherent light. Owing to its finite gap band structure, we find different mechanisms, including two-photon processes, might be responsible for the SSPM in MoS2 [with a large nonlinear dielectric susceptibility χ (3) = 1.6 × 10-9 e.s.u. (SI: 2.23 × 10-17 m2/V2) per layer]. Finally, we realized all optical switching based on SSPM, demonstrating that the electron coherence generation we report here is a ubiquitous property of layered quantum materials, by which novel optical applications are accessible. National Natural Science Foundation of China (11274372).

Condenser optics, partial coherence, and imaging for soft-x-ray projection lithography.

PubMed

Sommargren, G E; Seppala, L G

1993-12-01

A condenser system couples the radiation source to an imaging system, controlling the uniformity and partial coherence at the object, which ultimately affects the characteristics of the aerial image. A soft-x-ray projection lithography system based on a ring-field imaging system and a laser-produced plasma x-ray source places considerable constraints on the design of a condenser system. Two designs are proposed, critical illumination and Köhler illumination, each of which requires three mirrors and scanning for covering the entire ring field with the required uniformity and partial coherence. Images based on Hopkins' formulation of partially coherent imaging are simulated.

Ultrafast laser control of backward superfluorescence towards standoff sensing

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

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

2014-01-13

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

Coherent Dirac plasmons in topological insulators

NASA Astrophysics Data System (ADS)

Mondal, Richarj; Arai, Akira; Saito, Yuta; Fons, Paul; Kolobov, Alexander V.; Tominaga, Junji; Hase, Muneaki

2018-04-01

We explore the ultrafast reflectivity response from photo-generated coupled phonon-surface Dirac plasmons in Sb2Te3 topological insulators several quintuple layers thick. The transient coherent phonon spectra obtained at different time frames exhibit a Fano-like asymmetric line shape of the A1g 2 mode, which is attributed to quantum interference between continuumlike coherent Dirac plasmons and phonons. By analyzing the time-dependent asymmetric line shape using the two-temperature model (TTM), it was determined that a Fano-like resonance persisted up to ≈1 ps after photo excitation with a relaxation profile dominated by Gaussian decay at ≤200 fs. The asymmetry parameter could be well described by the TTM for ≥200 fs, therefore suggesting the coherence time of the Dirac plasmon is ≈200 fs.

Soft x-ray coherent diffraction imaging on magnetic nanostructures

NASA Astrophysics Data System (ADS)

Shi, Xiaowen; Lee, James; Mishra, Shrawan; Parks, Daniel; Tyliszczak, Tolek; Shapiro, David; Roy, Sujoy; Kevan, Steve; Stxm Team At Als Collaboration; Soft X-Ray Microscopy Group At Als Collaboration; Soft X-ray scattering at ALS, LBL Team

2014-03-01

Coherent soft X-rays diffraction imaging enable coherent magnetic resonance scattering at transition metal L-edge to be probed so that magnetic domains could be imaged with very high spatial resolution with phase contrast, reaching sub-10nm. One of the overwhelming advantages of using coherent X-rays is the ability to resolve phase contrast images with linearly polarized light with both phase and absorption contrast comparing to real-space imaging, which can only be studied with circularly polarized light with absorption contrast only. Here we report our first results on high-resolution of magnetic domains imaging of CoPd multilayer thin film with coherent soft X-ray ptychography method. We are aiming to resolve and understand magnetic domain wall structures with the highest obtainable resolution here at Advanced Light Source. In principle types of magnetic domain walls could be studied so that Neel or Bloch walls can be distinguished by imaging. This work at LBNL was supported by the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy (contract no. DE-AC02- 05CH11231).

Gain dynamics in a soft X-ray laser ampli er perturbed by a strong injected X-ray eld

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

Wang, Yong; Wang, Shoujun; Oliva, E

2014-01-01

Seeding soft X-ray plasma ampli ers with high harmonics has been demonstrated to generate high-brightness soft X-ray laser pulses with full spatial and temporal coherence. The interaction between the injected coherent eld and the swept-gain medium has been modelled. However, no exper- iment has been conducted to probe the gain dynamics when perturbed by a strong external seed eld. Here, we report the rst X-ray pump X-ray probe measurement of the nonlinear response of a plasma ampli er perturbed by a strong soft X-ray ultra-short pulse. We injected a sequence of two time-delayed high-harmonic pulses (l518.9 nm) into a collisionallymore » excited nickel-like molybdenum plasma to measure with femto-second resolution the gain depletion induced by the saturated ampli cation of the high-harmonic pump and its subsequent recovery. The measured fast gain recovery in 1.5 1.75 ps con rms the possibility to generate ultra-intense, fully phase-coherent soft X-ray lasers by chirped pulse ampli cation in plasma ampli ers.« 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.

Coherent quantum depletion of an interacting atom condensate

PubMed Central

Kira, M.

2015-01-01

Sufficiently strong interactions promote coherent quantum transitions in spite of thermalization and losses, which are the adversaries of delicate effects such as reversibility and correlations. In atomic Bose–Einstein condensates (BECs), strong atom–atom interactions can eject atoms from the BEC to the normal component, yielding quantum depletion instead of temperature depletion. A recent experiment has already been verified to overcome losses. Here I show that it also achieves coherent quantum-depletion dynamics in a BEC swept fast enough from weak to strong atom–atom interactions. The elementary coherent process first excites the normal component into a liquid state that evolves into a spherical shell state, where the atom occupation peaks at a finite momentum to shield 50% of the BEC atoms from annihilation. The identified coherent processes resemble ultrafast semiconductor excitations expanding the scope of BEC explorations to many-body non-equilibrium studies. PMID:25767044

Entanglement of atomic qubits using an optical frequency comb.

PubMed

Hayes, D; Matsukevich, D N; Maunz, P; Hucul, D; Quraishi, Q; Olmschenk, S; Campbell, W; Mizrahi, J; Senko, C; Monroe, C

2010-04-09

We demonstrate the use of an optical frequency comb to coherently control and entangle atomic qubits. A train of off-resonant ultrafast laser pulses is used to efficiently and coherently transfer population between electronic and vibrational states of trapped atomic ions and implement an entangling quantum logic gate with high fidelity. This technique can be extended to the high field regime where operations can be performed faster than the trap frequency. This general approach can be applied to more complex quantum systems, such as large collections of interacting atoms or molecules.

Effects of heat transfer and energy absorption in the ablation of biological tissues by pulsetrain-burst (>100 MHz) ultrafast laser processing

NASA Astrophysics Data System (ADS)

Forrester, Paul; Bol, Kieran; Lilge, Lothar; Marjoribanks, Robin

2006-09-01

Energy absorption and heat transfer are important factors for regulating the effects of ablation of biological tissues. Heat transfer to surrounding material may be desirable when ablating hard tissue, such as teeth or bone, since melting can produce helpful material modifications. However, when ablating soft tissue it is important to minimize heat transfer to avoid damage to healthy tissue - for example, in eye refractive surgery (e.g., Lasik), nanosecond pulses produce gross absorption and heating in tissue, leading to shockwaves, which kill and thin the non-replicating epithelial cells on the inside of the cornea; ultrafast pulses are recognized to reduce this effect. Using a laser system that delivers 1ps pulses in 10μs pulsetrains at 133MHz we have studied a range of heat- and energy-transfer effects on hard and soft tissue. We describe the ablation of tooth dentin and enamel under various conditions to determine the ablation rate and chemical changes that occur. Furthermore, we characterize the impact of pulsetrain-burst treatment of collagen-based tissue to determine more efficient methods of energy transfer to soft tissues. By studying the optical science of laser tissue interaction we hope to be able to make qualitative improvements to medical treatments using lasers.

Noncontact measurement of elasticity for the detection of soft-tissue tumors using phase-sensitive optical coherence tomography combined with a focused air-puff system.

PubMed

Wang, Shang; Li, Jiasong; Manapuram, Ravi Kiran; Menodiado, Floredes M; Ingram, Davis R; Twa, Michael D; Lazar, Alexander J; Lev, Dina C; Pollock, Raphael E; Larin, Kirill V

2012-12-15

We report on an optical noncontact method for the detection of soft-tissue tumors based on the measurement of their elasticity. A focused air-puff system is used to excite surface waves (SWs) on soft tissues with transient static pressure. A high-speed phase-sensitive optical coherence tomography system is used to measure the SWs as they propagate from the point of excitation. To evaluate the stiffness of soft tissues, the Young's modulus is quantified based on the group velocity of SWs. Pilot experiments were performed on ex vivo human myxoma and normal fat. Results demonstrate the feasibility of the proposed method to measure elasticity and differentiate soft-tissue tumors from normal tissues.

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

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

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

2006-08-07

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

Lattice-mediated magnetic order melting in TbMnO 3

DOE PAGES

Baldini, Edoardo; Kubacka, Teresa; Mallett, Benjamin P. P.; ...

2018-03-15

Recent ultrafast magnetic-sensitive measurements have revealed a delayed melting of the long-range cycloid spin order in TbMnO 3 following photoexcitation across the fundamental Mott-Hubbard gap. The microscopic mechanism behind this slow transfer of energy from the photoexcited carriers to the spin degrees of freedom is still elusive and not understood. Here, we address this problem by combining spectroscopic ellipsometry, ultrafast broadband optical spectroscopy, and ab initio calculations. Upon photoexcitation, we observe the emergence of a complex collective response, which is due to high-energy coherent optical phonons coupled to the out-of-equilibrium charge density. This response precedes the magnetic order melting andmore » is interpreted as the fingerprint of the formation of anti-Jahn-Teller polarons. We propose that the charge localization in a long-lived self-trapped state hinders the emission of magnons and other spin-flip mechanisms, causing the energy transfer from the charge to the spin system to be mediated by the reorganization of the lattice. In conclusion, we provide evidence for the coherent excitation of a phonon mode associated with the ferroelectric phase transition.« less

THz acoustic phonon spectroscopy and nanoscopy by using piezoelectric semiconductor heterostructures.

PubMed

Mante, Pierre-Adrien; Huang, Yu-Ru; Yang, Szu-Chi; Liu, Tzu-Ming; Maznev, Alexei A; Sheu, Jinn-Kong; Sun, Chi-Kuang

2015-02-01

Thanks to ultrafast acoustics, a better understanding of acoustic dynamics on a short time scale has been obtained and new characterization methods at the nanoscale have been developed. Among the materials that were studied during the development of ultrafast acoustics, nitride based heterostructures play a particular role due to their piezoelectric properties and the possibility to generate phonons with over-THz frequency and bandwidth. Here, we review some of the work performed using this type of structure, with a focus on THz phonon spectroscopy and nanoscopy. First, we present a brief description of the theory of coherent acoustic phonon generation by piezoelectric heterostructure. Then the first experimental observation of coherent acoustic phonon generated by the absorption of ultrashort light pulses in piezoelectric heterostructures is presented. From this starting point, we then present some methods developed to realize customizable phonon generation. Finally we review some more recent applications of these structures, including imaging with a nanometer resolution, broadband attenuation measurements with a frequency up to 1THz and phononic bandgap characterization. Copyright © 2014 Elsevier B.V. All rights reserved.

Lattice-mediated magnetic order melting in TbMnO 3

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

Baldini, Edoardo; Kubacka, Teresa; Mallett, Benjamin P. P.

Recent ultrafast magnetic-sensitive measurements have revealed a delayed melting of the long-range cycloid spin order in TbMnO 3 following photoexcitation across the fundamental Mott-Hubbard gap. The microscopic mechanism behind this slow transfer of energy from the photoexcited carriers to the spin degrees of freedom is still elusive and not understood. Here, we address this problem by combining spectroscopic ellipsometry, ultrafast broadband optical spectroscopy, and ab initio calculations. Upon photoexcitation, we observe the emergence of a complex collective response, which is due to high-energy coherent optical phonons coupled to the out-of-equilibrium charge density. This response precedes the magnetic order melting andmore » is interpreted as the fingerprint of the formation of anti-Jahn-Teller polarons. We propose that the charge localization in a long-lived self-trapped state hinders the emission of magnons and other spin-flip mechanisms, causing the energy transfer from the charge to the spin system to be mediated by the reorganization of the lattice. In conclusion, we provide evidence for the coherent excitation of a phonon mode associated with the ferroelectric phase transition.« less

Doppler-free spectroscopy of the atomic rubidium fine structure using ultrafast spatial coherent control method

NASA Astrophysics Data System (ADS)

Kim, Minhyuk; Kim, Kyungtae; Lee, Woojun; Kim, Hyosub; Ahn, Jaewook

2017-04-01

Spectral programming solutions for the ultrafast spatial coherent control (USCC) method to resolve the fine-structure energy levels of atomic rubidium are reported. In USCC, a pair of counter-propagating ultrashort laser pulses are programmed to make a two-photon excitation pattern specific to particular transition pathways and atom species, thus allowing the involved transitions resolvable in space simultaneously. With a proper spectral phase and amplitude modulation, USCC has been also demonstrated for the systems with many intermediate energy levels. Pushing the limit of system complexity even further, we show here an experimental demonstration of the rubidium fine-structure excitation pattern resolvable by USCC. The spectral programming solution for the given USCC is achieved by combining a double-V-shape spectral phase function and a set of phase steps, where the former distinguishes the fine structure and the latter prevents resonant transitions. The experimental results will be presented along with its application in conjunction with the Doppler-free frequency-comb spectroscopy for rubidium hyperfine structure measurements. Samsung Science and Technology Foundation [SSTFBA1301-12].

Suppression of quantum decoherence via infrared-driven coherent exciton-plasmon coupling: Undamped field and Rabi oscillations

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

Sadeghi, S. M., E-mail: seyed.sadeghi@uah.edu; Nano and Micro Device Center, University of Alabama in Huntsville, Huntsville, Alabama 35899; Patty, K. D.

2014-02-24

We show that when a semiconductor quantum dot is in the vicinity of a metallic nanoparticle and driven by a mid-infrared laser field, its coherent dynamics caused by interaction with a visible laser field can become free of quantum decoherence. We demonstrate that this process, which can offer undamped Rabi and field oscillations, is the result of coherent normalization of the “effective” polarization dephasing time of the quantum dot (T{sub 2}{sup *}). This process indicates formation of infrared-induced coherently forced oscillations, which allows us to control the value of T{sub 2}{sup *} using the infrared laser. The results offer decay-freemore » ultrafast modulation of the effective field experienced by the quantum dot when neither the visible laser field nor the infrared laser changes with time.« less

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.

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

PubMed

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

2008-11-13

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

Near-Infrared Chromophore Functionalized Soft Actuator with Ultrafast Photoresponsive Speed and Superior Mechanical Property.

PubMed

Liu, Li; Liu, Mei-Hua; Deng, Lin-Lin; Lin, Bao-Ping; Yang, Hong

2017-08-23

In this Communication, we develop a two-step acyclic diene metathesis in situ polymerization/cross-linking method to synthesize uniaxially aligned main-chain liquid crystal elastomers with chemically bonded near-infrared absorbing four-alkenyl-tailed croconaine-core cross-linkers. Because of the extraordinary photothermal conversion property, such a soft actuator material can raise its local temperature from 18 to 260 °C in 8 s, and lift up burdens 5600 times heavier than its own weight, under 808 nm near-infrared irradiation.

Electron diffraction using ultrafast electron bunches from a laser-wakefield accelerator at kHz repetition rate

NASA Astrophysics Data System (ADS)

He, Z.-H.; Thomas, A. G. R.; Beaurepaire, B.; Nees, J. A.; Hou, B.; Malka, V.; Krushelnick, K.; Faure, J.

2013-02-01

We show that electron bunches in the 50-100 keV range can be produced from a laser wakefield accelerator using 10 mJ, 35 fs laser pulses operating at 0.5 kHz. It is shown that using a solenoid magnetic lens, the electron bunch distribution can be shaped. The resulting transverse and longitudinal coherence is suitable for producing diffraction images from a polycrystalline 10 nm aluminum foil. The high repetition rate, the stability of the electron source, and the fact that its uncorrelated bunch duration is below 100 fs make this approach promising for the development of sub-100 fs ultrafast electron diffraction experiments.

Quantum modeling of ultrafast photoinduced charge separation

NASA Astrophysics Data System (ADS)

Rozzi, Carlo Andrea; Troiani, Filippo; Tavernelli, Ivano

2018-01-01

Phenomena involving electron transfer are ubiquitous in nature, photosynthesis and enzymes or protein activity being prominent examples. Their deep understanding thus represents a mandatory scientific goal. Moreover, controlling the separation of photogenerated charges is a crucial prerequisite in many applicative contexts, including quantum electronics, photo-electrochemical water splitting, photocatalytic dye degradation, and energy conversion. In particular, photoinduced charge separation is the pivotal step driving the storage of sun light into electrical or chemical energy. If properly mastered, these processes may also allow us to achieve a better command of information storage at the nanoscale, as required for the development of molecular electronics, optical switching, or quantum technologies, amongst others. In this Topical Review we survey recent progress in the understanding of ultrafast charge separation from photoexcited states. We report the state-of-the-art of the observation and theoretical description of charge separation phenomena in the ultrafast regime mainly focusing on molecular- and nano-sized solar energy conversion systems. In particular, we examine different proposed mechanisms driving ultrafast charge dynamics, with particular regard to the role of quantum coherence and electron-nuclear coupling, and link experimental observations to theoretical approaches based either on model Hamiltonians or on first principles simulations.

Ultrafast all-optical control of the magnetization in magnetic dielectrics

NASA Astrophysics Data System (ADS)

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

2006-08-01

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

Coherent and conventional gravidynamic quantum 1/f noise

NASA Astrophysics Data System (ADS)

Handel, Peter H.; George, Thomas F.

2008-04-01

Quantum 1/f noise is a fundamental fluctuation of currents, physical cross sections or process rates, caused by infrared coupling of the current carriers to very low frequency (soft) quanta, also known as infraquanta. The latter are soft gravitons in the gravidynamic case with the coupling constant g= pGM2/Nch considered here -- soft photons in the electrodynamic case and soft transversal piezo-phonons in the lattice-dynamical case. Here p=3.14 and F=psi. Quantum 1/f noise is a new aspect of quantum mechanics expressed mainly through the coherent quantum 1/f effect 2g/pf derived here for large systems, and mainly through the conventional quantum 1/f effect for small systems or individual particles. Both effects are present in general, and their effects are superposed in a first approximation with the help of a coherence (weight) parameter s" that will be derived elsewhere for the gravitational case. The spectral density of fractional fluctuations S(dj/j,f) for j=e(hk/2pm)|F|2 is S(F2,f)/<|F|2> = S(j,f)/2 = [4ps"/(1+s")]GM2/pfNch = 4.4 10E9 M2/(pfNgram2). Here s" = 2N'GM/c2=N'rs, where N' is the number of particles of mass M per unit length of the current, rs their Schwarzschild radius, and s" is our coherence (weight) parameter giving the ratio of coherent to conventional quantum 1/f contributions.

Current Trend Towards Using Soft Computing Approaches to Phase Synchronization in Communication Systems

NASA Technical Reports Server (NTRS)

Drake, Jeffrey T.; Prasad, Nadipuram R.

1999-01-01

This paper surveys recent advances in communications that utilize soft computing approaches to phase synchronization. Soft computing, as opposed to hard computing, is a collection of complementary methodologies that act in producing the most desirable control, decision, or estimation strategies. Recently, the communications area has explored the use of the principal constituents of soft computing, namely, fuzzy logic, neural networks, and genetic algorithms, for modeling, control, and most recently for the estimation of phase in phase-coherent communications. If the receiver in a digital communications system is phase-coherent, as is often the case, phase synchronization is required. Synchronization thus requires estimation and/or control at the receiver of an unknown or random phase offset.

Multiplane wave imaging increases signal-to-noise ratio in ultrafast ultrasound imaging.

PubMed

Tiran, Elodie; Deffieux, Thomas; Correia, Mafalda; Maresca, David; Osmanski, Bruno-Felix; Sieu, Lim-Anna; Bergel, Antoine; Cohen, Ivan; Pernot, Mathieu; Tanter, Mickael

2015-11-07

Ultrafast imaging using plane or diverging waves has recently enabled new ultrasound imaging modes with improved sensitivity and very high frame rates. Some of these new imaging modalities include shear wave elastography, ultrafast Doppler, ultrafast contrast-enhanced imaging and functional ultrasound imaging. Even though ultrafast imaging already encounters clinical success, increasing even more its penetration depth and signal-to-noise ratio for dedicated applications would be valuable. Ultrafast imaging relies on the coherent compounding of backscattered echoes resulting from successive tilted plane waves emissions; this produces high-resolution ultrasound images with a trade-off between final frame rate, contrast and resolution. In this work, we introduce multiplane wave imaging, a new method that strongly improves ultrafast images signal-to-noise ratio by virtually increasing the emission signal amplitude without compromising the frame rate. This method relies on the successive transmissions of multiple plane waves with differently coded amplitudes and emission angles in a single transmit event. Data from each single plane wave of increased amplitude can then be obtained, by recombining the received data of successive events with the proper coefficients. The benefits of multiplane wave for B-mode, shear wave elastography and ultrafast Doppler imaging are experimentally demonstrated. Multiplane wave with 4 plane waves emissions yields a 5.8  ±  0.5 dB increase in signal-to-noise ratio and approximately 10 mm in penetration in a calibrated ultrasound phantom (0.7 d MHz(-1) cm(-1)). In shear wave elastography, the same multiplane wave configuration yields a 2.07  ±  0.05 fold reduction of the particle velocity standard deviation and a two-fold reduction of the shear wave velocity maps standard deviation. In functional ultrasound imaging, the mapping of cerebral blood volume results in a 3 to 6 dB increase of the contrast-to-noise ratio in deep structures of the rodent brain.

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

PubMed

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

2013-01-01

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

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

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.

Realizing Ultrafast Electron Pulse Self-Compression by Femtosecond Pulse Shaping Technique.

PubMed

Qi, Yingpeng; Pei, Minjie; Qi, Dalong; Yang, Yan; Jia, Tianqing; Zhang, Shian; Sun, Zhenrong

2015-10-01

Uncorrelated position and velocity distribution of the electron bunch at the photocathode from the residual energy greatly limit the transverse coherent length and the recompression ability. Here we first propose a femtosecond pulse-shaping method to realize the electron pulse self-compression in ultrafast electron diffraction system based on a point-to-point space-charge model. The positively chirped femtosecond laser pulse can correspondingly create the positively chirped electron bunch at the photocathode (such as metal-insulator heterojunction), and such a shaped electron pulse can realize the self-compression in the subsequent propagation process. The greatest advantage for our proposed scheme is that no additional components are introduced into the ultrafast electron diffraction system, which therefore does not affect the electron bunch shape. More importantly, this scheme can break the limitation that the electron pulse via postphotocathode static compression schemes is not shorter than the excitation laser pulse due to the uncorrelated position and velocity distribution of the initial electron bunch.

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

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.

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

PubMed

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

2008-11-21

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

Characterization and imaging of nanostructured materials using tabletop extreme ultraviolet light sources

NASA Astrophysics Data System (ADS)

Karl, Robert; Knobloch, Joshua; Frazer, Travis; Tanksalvala, Michael; Porter, Christina; Bevis, Charles; Chao, Weilun; Abad Mayor, Begoña.; Adams, Daniel; Mancini, Giulia F.; Hernandez-Charpak, Jorge N.; Kapteyn, Henry; Murnane, Margaret

2018-03-01

Using a tabletop coherent extreme ultraviolet source, we extend current nanoscale metrology capabilities with applications spanning from new models of nanoscale transport and materials, to nanoscale device fabrication. We measure the ultrafast dynamics of acoustic waves in materials; by analyzing the material's response, we can extract elastic properties of films as thin as 11nm. We extend this capability to a spatially resolved imaging modality by using coherent diffractive imaging to image the acoustic waves in nanostructures as they propagate. This will allow for spatially resolved characterization of the elastic properties of non-isotropic materials.

40 MHz high-frequency ultrafast ultrasound imaging.

PubMed

Huang, Chih-Chung; Chen, Pei-Yu; Peng, Po-Hsun; Lee, Po-Yang

2017-06-01

Ultrafast high-frame-rate ultrasound imaging based on coherent-plane-wave compounding has been developed for many biomedical applications. Most coherent-plane-wave compounding systems typically operate at 3-15 MHz, and the image resolution for this frequency range is not sufficient for visualizing microstructure tissues. Therefore, the purpose of this study was to implement a high-frequency ultrafast ultrasound imaging operating at 40 MHz. The plane-wave compounding imaging and conventional multifocus B-mode imaging were performed using the Field II toolbox of MATLAB in simulation study. In experiments, plane-wave compounding images were obtained from a 256 channel ultrasound research platform with a 40 MHz array transducer. All images were produced by point-spread functions and cyst phantoms. The in vivo experiment was performed from zebrafish. Since high-frequency ultrasound exhibits a lower penetration, chirp excitation was applied to increase the imaging depth in simulation. The simulation results showed that a lateral resolution of up to 66.93 μm and a contrast of up to 56.41 dB were achieved when using 75-angles plane waves in compounding imaging. The experimental results showed that a lateral resolution of up to 74.83 μm and a contrast of up to 44.62 dB were achieved when using 75-angles plane waves in compounding imaging. The dead zone and compounding noise are about 1.2 mm and 2.0 mm in depth for experimental compounding imaging, respectively. The structure of zebrafish heart was observed clearly using plane-wave compounding imaging. The use of fewer than 23 angles for compounding allowed a frame rate higher than 1000 frames per second. However, the compounding imaging exhibits a similar lateral resolution of about 72 μm as the angle of plane wave is higher than 10 angles. This study shows the highest operational frequency for ultrafast high-frame-rate ultrasound imaging. © 2017 American Association of Physicists in Medicine.

Fourier ptychographic microscopy at telecommunication wavelengths using a femtosecond laser

NASA Astrophysics Data System (ADS)

Ahmed, Ishtiaque; Alotaibi, Maged; Skinner-Ramos, Sueli; Dominguez, Daniel; Bernussi, Ayrton A.; de Peralta, Luis Grave

2017-12-01

We report the implementation of the Fourier Ptychographic Microscopy (FPM) technique, a phase retrieval technique, at telecommunication wavelengths using a low-coherence ultrafast pulsed laser source. High quality images, near speckle-free, were obtained with the proposed approach. We demonstrate that FPM can also be used to image periodic features through a silicon wafer.

Ultra-short wavelength x-ray system

DOEpatents

Umstadter, Donald [Ann Arbor, MI; He, Fei [Ann Arbor, MI; Lau, Yue-Ying [Potomac, MD

2008-01-22

A method and apparatus to generate a beam of coherent light including x-rays or XUV by colliding a high-intensity laser pulse with an electron beam that is accelerated by a synchronized laser pulse. Applications include x-ray and EUV lithography, protein structural analysis, plasma diagnostics, x-ray diffraction, crack analysis, non-destructive testing, surface science and ultrafast science.

Theoretical Investigation of Optical Detection and Recognition of Single Biological Molecules Using Coherent Dynamics of Exciton-Plasmon Coupling

PubMed Central

Sadeghi, S. M.; Hood, B.; Patty, K. D.; Mao, C.-B.

2013-01-01

We use quantum coherence in a system consisting of one metallic nanorod and one semi-conductor quantum dot to investigate a plasmonic nanosensor capable of digital optical detection and recognition of single biological molecules. In such a sensor the adsorption of a specific molecule to the nanorod turns off the emission of the system when it interacts with an optical pulse having a certain intensity and temporal width. The proposed quantum sensors can count the number of molecules of the same type or differentiate between molecule types with digital optical signals that can be measured with high certainty. We show that these sensors are based on the ultrafast upheaval of coherent dynamics of the system and the removal of coherent blockage of energy transfer from the quantum dot to the nanorod once the adsorption process has occurred. PMID:24040424

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

NASA Astrophysics Data System (ADS)

Olivucci, Massimo

2014-03-01

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

Practical witness for electronic coherences

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

Johnson, Allan S.; Department of Physics, Imperial College London, London; Yuen-Zhou, Joel

2014-12-28

The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently, it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond exclusively to electronic coherences, and thus such experiments can be used to form a test for electronic vs. vibrational oscillations in such systems. Here, we demonstrate a method for practically implementing such a test, whereby pump-probe signals are taken at several different pulse durations and used to extrapolate to the ultrashort-pulse limit. We present analytic and numerical results determining requirements for pulse durations and the optimal choice of pulse centralmore » frequency, which can be determined from an absorption spectrum. Our results suggest that for numerous systems, the required experiment could be implemented by many ultrafast spectroscopy laboratories using pulses of tens of femtoseconds in duration. Such experiments could resolve the standing debate over the nature of coherences in photosynthetic complexes.« less

Femtosecond study of A1g phonons in the strong 3D topological insulators: From pump-probe to coherent control

NASA Astrophysics Data System (ADS)

Hu, Jianbo; Igarashi, Kyushiro; Sasagawa, Takao; Nakamura, Kazutaka G.; Misochko, Oleg V.

2018-01-01

Fully symmetric A1g phonons are expected to play a dominant role in electron scattering in strong topological insulators (TIs), thus limiting the ballistic transport of future electronic devices. Here, we report on femtosecond time-resolved observation of a pair of A1g coherent phonons and their optical control in two strong 3D TIs, Bi2Te3 and Bi2Se3, by using a second pump pulse in ultrafast spectroscopy measurements. Along with well-defined phonon properties such as frequency and lifetime, an obvious phonon chirp has been observed, implying a strong coupling between photo-carriers and lattices. The coherent phonon manipulation, on the other hand, allows us to change the phonon amplitude selectively but does not affect either the frequency or coherence lifetime of the chosen mode.

Practical witness for electronic coherences.

PubMed

Johnson, Allan S; Yuen-Zhou, Joel; Aspuru-Guzik, Alán; Krich, Jacob J

2014-12-28

The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently, it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond exclusively to electronic coherences, and thus such experiments can be used to form a test for electronic vs. vibrational oscillations in such systems. Here, we demonstrate a method for practically implementing such a test, whereby pump-probe signals are taken at several different pulse durations and used to extrapolate to the ultrashort-pulse limit. We present analytic and numerical results determining requirements for pulse durations and the optimal choice of pulse central frequency, which can be determined from an absorption spectrum. Our results suggest that for numerous systems, the required experiment could be implemented by many ultrafast spectroscopy laboratories using pulses of tens of femtoseconds in duration. Such experiments could resolve the standing debate over the nature of coherences in photosynthetic complexes.

Harmonic Quantum Coherence of Multiple Excitons in PbS/CdS Core-Shell Nanocrystals

NASA Astrophysics Data System (ADS)

Tahara, Hirokazu; Sakamoto, Masanori; Teranishi, Toshiharu; Kanemitsu, Yoshihiko

2017-12-01

The generation and recombination dynamics of multiple excitons in nanocrystals (NCs) have attracted much attention from the viewpoints of fundamental physics and device applications. However, the quantum coherence of multiple exciton states in NCs still remains unclear due to a lack of experimental support. Here, we report the first observation of harmonic dipole oscillations in PbS/CdS core-shell NCs using a phase-locked interference detection method for transient absorption. From the ultrafast coherent dynamics and excitation-photon-fluence dependence of the oscillations, we found that multiple excitons cause the harmonic dipole oscillations with ω , 2 ω , and 3 ω oscillations, even though the excitation pulse energy is set to the exciton resonance frequency, ω . This observation is closely related to the quantum coherence of multiple exciton states in NCs, providing important insights into multiple exciton generation mechanisms.

Generation of Bright, Spatially Coherent Soft X-Ray High Harmonics in a Hollow Waveguide Using Two-Color Synthesized Laser Pulses.

PubMed

Jin, Cheng; Stein, Gregory J; Hong, Kyung-Han; Lin, C D

2015-07-24

We investigate the efficient generation of low-divergence high-order harmonics driven by waveform-optimized laser pulses in a gas-filled hollow waveguide. The drive waveform is obtained by synthesizing two-color laser pulses, optimized such that highest harmonic yields are emitted from each atom. Optimization of the gas pressure and waveguide configuration has enabled us to produce bright and spatially coherent harmonics extending from the extreme ultraviolet to soft x rays. Our study on the interplay among waveguide mode, atomic dispersion, and plasma effect uncovers how dynamic phase matching is accomplished and how an optimized waveform is maintained when optimal waveguide parameters (radius and length) and gas pressure are identified. Our analysis should help laboratory development in the generation of high-flux bright coherent soft x rays as tabletop light sources for applications.

Temperature effect on the coupling between coherent longitudinal phonons and plasmons in n -type and p -type GaAs

NASA Astrophysics Data System (ADS)

Hu, Jianbo; Zhang, Hang; Sun, Yi; Misochko, Oleg V.; Nakamura, Kazutaka G.

2018-04-01

The coupling between longitudinal optical (LO) phonons and plasmons plays a fundamental role in determining the performance of doped semiconductor devices. In this work, we report a comparative investigation into the dependence of the coupling on temperature and doping in n - and p -type GaAs by using ultrafast coherent phonon spectroscopy. A suppression of coherent oscillations has been observed in p -type GaAs at lower temperature, strikingly different from n -type GaAs and other materials in which coherent oscillations are strongly enhanced by cooling. We attribute this unexpected observation to a cooling-induced elongation of the depth of the depletion layer which effectively increases the screening time of the surface field due to a slow diffusion of photoexcited carriers in p -type GaAs. Such an increase breaks the requirement for the generation of coherent LO phonons and, in turn, LO phonon-plasmon coupled modes because of their delayed formation in time.

Ultrafast frequency-selective optical switching based on thin self-assembled organic chromophoric films with a large second-order nonlinear response

NASA Astrophysics Data System (ADS)

Wang, Gang; Zhu, Peiwang; Marks, Tobin J.; Ketterson, J. B.

2002-09-01

Thin films consisting of self-assembled chromophoric superlattices exhibit very large second-order nonlinear responses [chi](2). Using such films, a "static" diffraction grating is created by the interference of two coherent infrared beams from a pulsed yttritium-aluminum-garnet laser. This grating is used to switch the second-harmonic and third-harmonic "signal" beams (generated from the fundamental "pump" beam or mixed within the chromophoric superlattice) into different channels (directions). Ultrafast switching response as a function of the time overlap of the pumping beams is demonstrated. It is suggested that such devices can be used to spatially and temporally separate signal trains consisting of pulses having different frequencies and arrival times.

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

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

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

2006-05-15

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

Contactless remote induction of shear waves in soft tissues using a transcranial magnetic stimulation device

NASA Astrophysics Data System (ADS)

Grasland-Mongrain, Pol; Miller-Jolicoeur, Erika; Tang, An; Catheline, Stefan; Cloutier, Guy

2016-03-01

This study presents the first observation of shear waves induced remotely within soft tissues. It was performed through the combination of a transcranial magnetic stimulation device and a permanent magnet. A physical model based on Maxwell and Navier equations was developed. Experiments were performed on a cryogel phantom and a chicken breast sample. Using an ultrafast ultrasound scanner, shear waves of respective amplitudes of 5 and 0.5 μm were observed. Experimental and numerical results were in good agreement. This study constitutes the framework of an alternative shear wave elastography method.

Ultrafast High Harmonic, Soft X-Ray Probing of Molecular Dynamics

DTIC Science & Technology

2009-12-16

12. D. G. Lappas and A. L’Huillier, "Generation of attosecond XUV pulses in strong laser-atom interactions," Phys. Rev. A 58, 4140 (1998). 13...presentation at the 37 th AIAA/ASME/ SAE /ASEE Joint Propulsion Conference and Exhibition, Salt Lake City, UT, p. 3937 (2001). 36. A. Bultel, B. G

Observation of antiphase coherent phonons in the warped Dirac cone of Bi2Te3

NASA Astrophysics Data System (ADS)

Golias, E.; Sánchez-Barriga, J.

2016-10-01

In this Rapid Communication we investigate the coupling between excited electrons and phonons in the highly anisotropic electronic structure of the prototypical topological insulator Bi2Te3 . Using time- and angle-resolved photoemission spectroscopy we are able to identify the emergence and ultrafast temporal evolution of the longitudinal-optical A1 g coherent-phonon mode in Bi2Te3 . We observe an antiphase behavior in the onset of the coherent-phonon oscillations between the Γ K ¯ and the Γ M ¯ high-symmetry directions that is consistent with warping. The qualitative agreement between our density-functional theory calculations and the experimental results reveals the critical role of the anisotropic coupling between Dirac fermions and phonon modes in the topological insulator Bi2Te3 .

CSR Fields: Direct Numerical Solution of the Maxwell___s Equation

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

Novokhatski, A.; /SLAC

2011-06-22

We discuss the properties of the coherent electromagnetic fields of a very short, ultra-relativistic bunch in a rectangular vacuum chamber inside a bending magnet. The analysis is based on the results of a direct numerical solution of Maxwell's equations together with Newton's equations. We use a new dispersion-free time-domain algorithm which employs a more efficient use of finite element mesh techniques and hence produces self-consistent and stable solutions for very short bunches. We investigate the fine structure of the CSR fields including coherent edge radiation. This approach should be useful in the study of existing and future concepts of particlemore » accelerators and ultrafast coherent light sources. The coherent synchrotron radiation (CSR) fields have a strong action on the beam dynamics of very short bunches, which are moving in the bends of all kinds of magnetic elements. They are responsible for additional energy loss and energy spread; micro bunching and beam emittance growth. These fields may bound the efficiency of damping rings, electron-positron colliders and ultrafast coherent light sources, where high peak currents and very short bunches are envisioned. This is relevant to most high-brightness beam applications. On the other hand these fields together with transition radiation fields can be used for beam diagnostics or even as a powerful resource of THz radiation. A history of the study of CSR and a good collection of references can be found in [1]. Electromagnetic theory suggests several methods on how to calculate CSR fields. The most popular method is to use Lienard-Wiechert potentials. Other approach is to solve numerically the approximate equations, which are a Schrodinger type equation. These numerical methods are described in [2]. We suggest that a direct solution of Maxwell's equations together with Newton's equations can describe the detailed structure of the CSR fields [3].« less

Ultrafast Synthetic Transmit Aperture Imaging Using Hadamard-Encoded Virtual Sources With Overlapping Sub-Apertures.

PubMed

Ping Gong; Pengfei Song; Shigao Chen

2017-06-01

The development of ultrafast ultrasound imaging offers great opportunities to improve imaging technologies, such as shear wave elastography and ultrafast Doppler imaging. In ultrafast imaging, there are tradeoffs among image signal-to-noise ratio (SNR), resolution, and post-compounded frame rate. Various approaches have been proposed to solve this tradeoff, such as multiplane wave imaging or the attempts of implementing synthetic transmit aperture imaging. In this paper, we propose an ultrafast synthetic transmit aperture (USTA) imaging technique using Hadamard-encoded virtual sources with overlapping sub-apertures to enhance both image SNR and resolution without sacrificing frame rate. This method includes three steps: 1) create virtual sources using sub-apertures; 2) encode virtual sources using Hadamard matrix; and 3) add short time intervals (a few microseconds) between transmissions of different virtual sources to allow overlapping sub-apertures. The USTA was tested experimentally with a point target, a B-mode phantom, and in vivo human kidney micro-vessel imaging. Compared with standard coherent diverging wave compounding with the same frame rate, improvements on image SNR, lateral resolution (+33%, with B-mode phantom imaging), and contrast ratio (+3.8 dB, with in vivo human kidney micro-vessel imaging) have been achieved. The f-number of virtual sources, the number of virtual sources used, and the number of elements used in each sub-aperture can be flexibly adjusted to enhance resolution and SNR. This allows very flexible optimization of USTA for different applications.

Advanced Instrumentation for Ultrafast Science at the LCLS

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

Berrah, Nora

2015-10-13

This grant supported a Single Investigator and Small Group Research (SISGR) application to enable multi-user research in Ultrafast Science using the Linac Coherent Light Source (LCLS), the world’s first hard x-ray free electron laser (FEL) which lased for the first time at 1.5 Å on April 20, 2009. The goal of our proposal was to enable a New Era of Science by requesting funds to purchase and build Advanced Instrumentation for Ultrafast Science (AIUS), to utilize the intense, short x-ray pulses produced by the LCLS. The proposed instrumentation will allow peer review selected users to probe the ultrasmall and capture themore » ultrafast. These tools will expand on the investment already made in the construction of the light source and its instrumentation in both the LCLS and LUSI projects. The AIUS will provide researchers in the AMO, Chemical, Biological and Condensed Matter communities with greater flexibility in defining their scientific agenda at the LCLS. The proposed instrumentation will complement and significantly augment the present AMO instrument (funded through the LCLS project) through detectors and capabilities not included in the initial suite of instrumentation at the facility. We have built all of the instrumentations and they have been utilized by scientists. Please see report attached.« less

Breaking resolution limits in ultrafast electron diffraction and microscopy.

PubMed

Baum, Peter; Zewail, Ahmed H

2006-10-31

Ultrafast electron microscopy and diffraction are powerful techniques for the study of the time-resolved structures of molecules, materials, and biological systems. Central to these approaches is the use of ultrafast coherent electron packets. The electron pulses typically have an energy of 30 keV for diffraction and 100-200 keV for microscopy, corresponding to speeds of 33-70% of the speed of light. Although the spatial resolution can reach the atomic scale, the temporal resolution is limited by the pulse width and by the difference in group velocities of electrons and the light used to initiate the dynamical change. In this contribution, we introduce the concept of tilted optical pulses into diffraction and imaging techniques and demonstrate the methodology experimentally. These advances allow us to reach limits of time resolution down to regimes of a few femtoseconds and, possibly, attoseconds. With tilted pulses, every part of the sample is excited at precisely the same time as when the electrons arrive at the specimen. Here, this approach is demonstrated for the most unfavorable case of ultrafast crystallography. We also present a method for measuring the duration of electron packets by autocorrelating electron pulses in free space and without streaking, and we discuss the potential of tilting the electron pulses themselves for applications in domains involving nuclear and electron motions.

Temperature dependent of IVR investigated by steady-state and time-frequency resolved CARS for liquid nitrobenzene and nitromethane

NASA Astrophysics Data System (ADS)

Yang, Yanqiang; Zhu, Gangbei; Yan, Lin; Liu, Xiaosong; Yang's Ultrafast Spectroscopy Group Team

2017-06-01

Intramolecular vibrational energy redistribution (IVR) is important process in thermal decomposition, shock chemistry and photochemistry. Anti-Stokes Raman scattering is sensitive to the vibrational population in excited states because only vibrational excited states are responsible to the anti-Stokes Raman scattering, does not vibrational ground states. In this report, steady-state anti-Stokes Raman spectroscopy and broad band ultrafast coherent anti-Stokes Raman scattering (CARS) are performed. The steady-state anti-Stokes Raman spectroscopy shows temperature dependent of vibrational energy redistribution in vibrational excited-state molecule, and reveal that, in liquid nitrobenzene, with temperature increasing, vibrational energy is mainly redistributed in NO2 symmetric stretching mode, and phenyl ring stretching mode of νCC. For liquid nitromethane, it is found that, with temperature increasing, vibrational energy concentrate in CN stretching mode and methyl umbrella vibrational mode. In the broad band ultrafast CARS experiment, multiple vibrational modes are coherently excited to vibrational excited states, and the time-frequency resolved CARS spectra show the coincident IVR processes. This work is supported by the National Natural Science Foundation of China (Grant Numbers 21673211 and 11372053), and the Science Challenging Program (Grant Number JCKY2016212A501).

Laser acceleration

NASA Astrophysics Data System (ADS)

Tajima, T.; Nakajima, K.; Mourou, G.

2017-02-01

The fundamental idea of Laser Wakefield Acceleration (LWFA) is reviewed. An ultrafast intense laser pulse drives coherent wakefield with a relativistic amplitude robustly supported by the plasma. While the large amplitude of wakefields involves collective resonant oscillations of the eigenmode of the entire plasma electrons, the wake phase velocity ˜ c and ultrafastness of the laser pulse introduce the wake stability and rigidity. A large number of worldwide experiments show a rapid progress of this concept realization toward both the high-energy accelerator prospect and broad applications. The strong interest in this has been spurring and stimulating novel laser technologies, including the Chirped Pulse Amplification, the Thin Film Compression, the Coherent Amplification Network, and the Relativistic Mirror Compression. These in turn have created a conglomerate of novel science and technology with LWFA to form a new genre of high field science with many parameters of merit in this field increasing exponentially lately. This science has triggered a number of worldwide research centers and initiatives. Associated physics of ion acceleration, X-ray generation, and astrophysical processes of ultrahigh energy cosmic rays are reviewed. Applications such as X-ray free electron laser, cancer therapy, and radioisotope production etc. are considered. A new avenue of LWFA using nanomaterials is also emerging.

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.

Phase-space foundations of electron holography

NASA Astrophysics Data System (ADS)

Lubk, A.; Röder, F.

2015-09-01

We present a unified formalism for describing various forms of electron holography in quantum mechanical phase space including their extensions to quantum-state reconstructions. The phase-space perspective allows for taking into account partial coherence as well as the quantum mechanical detection process typically hampering the unique reconstruction of a wave function. We elaborate on the limitations imposed by the electron optical elements of the transmission electron microscope as well as the scattering at the target. The results provide the basis for vastly extending the scope of electron holographic techniques towards analyzing partially coherent signals such as inelastically scattered electrons or electron pulses used in ultrafast transmission electron microscopy.

Bright broadband coherent fiber sources emitting strongly blue-shifted resonant dispersive wave pulses

PubMed Central

Tu, Haohua; Lægsgaard, Jesper; Zhang, Rui; Tong, Shi; Liu, Yuan; Boppart, Stephen A.

2013-01-01

We predict and realize the targeted wavelength conversion from the 1550-nm band of a fs Er:fiber laser to an isolated band inside 370-850 nm, corresponding to a blue-shift of 700-1180 nm. The conversion utilizes resonant dispersive wave generation in widely available optical fibers with good efficiency (~7%). The converted band has a large pulse energy (~1 nJ), high spectral brightness (~1 mW/nm), and broad Gaussian-like spectrum compressible to clean transform-limited ~17 fs pulses. The corresponding coherent fiber sources open up portable applications of optical parametric oscillators and dual-output synchronized ultrafast lasers. PMID:24104233

Engineering nanometre-scale coherence in soft matter

NASA Astrophysics Data System (ADS)

Liu, Chaoren; Xiang, Limin; Zhang, Yuqi; Zhang, Peng; Beratan, David N.; Li, Yueqi; Tao, Nongjian

2016-10-01

Electronic delocalization in redox-active polymers may be disrupted by the heterogeneity of the environment that surrounds each monomer. When the differences in monomer redox-potential induced by the environment are small (as compared with the monomer-monomer electronic interactions), delocalization persists. Here we show that guanine (G) runs in double-stranded DNA support delocalization over 4-5 guanine bases. The weak interaction between delocalized G blocks on opposite DNA strands is known to support partially coherent long-range charge transport. The molecular-resolution model developed here finds that the coherence among these G blocks follows an even-odd orbital-symmetry rule and predicts that weakening the interaction between G blocks exaggerates the resistance oscillations. These findings indicate how sequence can be exploited to change the balance between coherent and incoherent transport. The predictions are tested and confirmed using break-junction experiments. Thus, tailored orbital symmetry and structural fluctuations may be used to produce coherent transport with a length scale of multiple nanometres in soft-matter assemblies, a length scale comparable to that of small proteins.

Measurement of Shear Elastic Moduli in Quasi-Incompressible Soft Solids

NASA Astrophysics Data System (ADS)

Rénier, Mathieu; Gennisson, Jean-Luc; Barrière, Christophe; Catheline, Stefan; Tanter, Mickaël; Royer, Daniel; Fink, Mathias

2008-06-01

Recently a nonlinear equation describing the plane shear wave propagation in isotropic quasi-incompressible media has been developed using a new expression of the strain energy density, as a function of the second, third and fourth order shear elastic constants (respectively μ, A, D) [1]. In such a case, the shear nonlinearity parameter βs depends only from these last coefficients. To date, no measurement of the parameter D have been carried out in soft solids. Using a set of two experiments, acoustoelasticity and finite amplitude shear waves, the shear elastic moduli up to the fourth order of soft solids are measured. Firstly, this theoretical background is applied to the acoustoelasticity theory, giving the variations of the shear wave speed as a function of the stress applied to the medium. From such variations, both linear (μ) and third order shear modulus (A) are deduced in agar-gelatin phantoms. Experimentally the radiation force induced by a focused ultrasound beam is used to generate quasi-plane linear shear waves within the medium. Then the shear wave propagation is imaged with an ultrafast ultrasound scanner. Secondly, in order to give rise to finite amplitude plane shear waves, the radiation force generation technique is replaced by a vibrating plate applied at the surface of the phantoms. The propagation is also imaged using the same ultrafast scanner. From the assessment of the third harmonic amplitude, the nonlinearity parameter βS is deduced. Finally, combining these results with the acoustoelasticity experiment, the fourth order modulus (D) is deduced. This set of experiments provides the characterization, up to the fourth order, of the nonlinear shear elastic moduli in quasi-incompressible soft media. Measurements of the A moduli reveal that while the behaviors of both soft solids are close from a linear point of view, the corresponding nonlinear moduli A are quite different. In a 5% agar-gelatin phantom, the fourth order elastic constant D is found to be 30±10 kPa.

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

NASA Astrophysics Data System (ADS)

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

2012-04-01

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

Ultrafast electronic dynamics driven by nuclear motion

NASA Astrophysics Data System (ADS)

Vendrell, Oriol

2016-05-01

The transfer of electrical charge on a microscopic scale plays a fundamental role in chemistry, in biology, and in technological applications. In this contribution, we will discuss situations in which nuclear motion plays a central role in driving the electronic dynamics of photo-excited or photo-ionized molecular systems. In particular, we will explore theoretically the ultrafast transfer of a double electron hole between the functional groups of glycine after K-shell ionization and subsequent Auger decay. Although a large energy gap of about 15 eV initially exists between the two electronic states involved and coherent electronic dynamics play no role in the hole transfer, we will illustrate how the double hole can be transferred within 3 to 4 fs between both functional ends of the glycine molecule driven solely by specific nuclear displacements and non-Born-Oppenheimer effects. This finding challenges the common wisdom that nuclear dynamics of the molecular skeleton are unimportant for charge transfer processes at the few-femtosecond time scale and shows that they can even play a prominent role. We thank the Hamburg Centre for Ultrafast Imaging and the Volkswagen Foundation for financial support.

Ultrafast adiabatic quantum algorithm for the NP-complete exact cover problem

PubMed Central

Wang, Hefeng; Wu, Lian-Ao

2016-01-01

An adiabatic quantum algorithm may lose quantumness such as quantum coherence entirely in its long runtime, and consequently the expected quantum speedup of the algorithm does not show up. Here we present a general ultrafast adiabatic quantum algorithm. We show that by applying a sequence of fast random or regular signals during evolution, the runtime can be reduced substantially, whereas advantages of the adiabatic algorithm remain intact. We also propose a randomized Trotter formula and show that the driving Hamiltonian and the proposed sequence of fast signals can be implemented simultaneously. We illustrate the algorithm by solving the NP-complete 3-bit exact cover problem (EC3), where NP stands for nondeterministic polynomial time, and put forward an approach to implementing the problem with trapped ions. PMID:26923834

Transverse Coherence Limited Coherent Diffraction Imaging using a Molybdenum Soft X-ray Laser Pumped at Moderate Pump Energies.

PubMed

Zürch, M; Jung, R; Späth, C; Tümmler, J; Guggenmos, A; Attwood, D; Kleineberg, U; Stiel, H; Spielmann, C

2017-07-13

Coherent diffraction imaging (CDI) in the extreme ultraviolet has become an important tool for nanoscale investigations. Laser-driven high harmonic generation (HHG) sources allow for lab scale applications such as cancer cell classification and phase-resolved surface studies. HHG sources exhibit excellent coherence but limited photon flux due poor conversion efficiency. In contrast, table-top soft X-ray lasers (SXRL) feature excellent temporal coherence and extraordinary high flux at limited transverse coherence. Here, the performance of a SXRL pumped at moderate pump energies is evaluated for CDI and compared to a HHG source. For CDI, a lower bound for the required mutual coherence factor of |μ 12 | ≥ 0.75 is found by comparing a reconstruction with fixed support to a conventional characterization using double slits. A comparison of the captured diffraction signals suggests that SXRLs have the potential for imaging micron scale objects with sub-20 nm resolution in orders of magnitude shorter integration time compared to a conventional HHG source. Here, the low transverse coherence diameter limits the resolution to approximately 180 nm. The extraordinary high photon flux per laser shot, scalability towards higher repetition rate and capability of seeding with a high harmonic source opens a route for higher performance nanoscale imaging systems based on SXRLs.

Spatial-temporal ultrasound imaging of residual cavitation bubbles around a fluid-tissue interface in histotripsy.

PubMed

Hu, Hong; Xu, Shanshan; Yuan, Yuan; Liu, Runna; Wang, Supin; Wan, Mingxi

2015-05-01

Cavitation is considered as the primary mechanism of soft tissue fragmentation (histotripsy) by pulsed high-intensity focused ultrasound. The residual cavitation bubbles have a dual influence on the histotripsy pulses: these serve as nuclei for easy generation of new cavitation, and act as strong scatterers causing energy "shadowing." To monitor the residual cavitation bubbles in histotripsy, an ultrafast active cavitation imaging method with relatively high signal-to-noise ratio and good spatial-temporal resolution was proposed in this paper, which combined plane wave transmission, minimum variance beamforming, and coherence factor weighting. The spatial-temporal evolutions of residual cavitation bubbles around a fluid-tissue interface in histotripsy under pulse duration (PD) of 10-40 μs and pulse repetition frequency (PRF) of 0.67-2 kHz were monitored by this method. The integrated bubble area curves inside the tissue interface were acquired from the bubble image sequence, and the formation process of histotripsy damage was estimated. It was observed that the histotripsy efficiency decreased with both longer PDs and higher PRFs. A direct relationship with a coefficient of 1.0365 between histotripsy lesion area and inner residual bubble area was found. These results can assist in monitoring and optimization of the histotripsy treatment further.

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. Finally, a new inverse transform procedure is presented that calculates the absorption band (ABS) from an experimental Raman excitation profile (REP). An iterative solution is sought for an integral Hilbert transform relation. An exact ABS is recovered regardless of the starting ABS when sufficient iterations are performed.

Coherent soft X-ray diffraction imaging of coliphage PR772 at the Linac coherent light source

PubMed Central

Reddy, Hemanth K.N.; Yoon, Chun Hong; Aquila, Andrew; Awel, Salah; Ayyer, Kartik; Barty, Anton; Berntsen, Peter; Bielecki, Johan; Bobkov, Sergey; Bucher, Maximilian; Carini, Gabriella A.; Carron, Sebastian; Chapman, Henry; Daurer, Benedikt; DeMirci, Hasan; Ekeberg, Tomas; Fromme, Petra; Hajdu, Janos; Hanke, Max Felix; Hart, Philip; Hogue, Brenda G.; Hosseinizadeh, Ahmad; Kim, Yoonhee; Kirian, Richard A.; Kurta, Ruslan P.; Larsson, Daniel S.D.; Duane Loh, N.; Maia, Filipe R.N.C.; Mancuso, Adrian P.; Mühlig, Kerstin; Munke, Anna; Nam, Daewoong; Nettelblad, Carl; Ourmazd, Abbas; Rose, Max; Schwander, Peter; Seibert, Marvin; Sellberg, Jonas A.; Song, Changyong; Spence, John C.H.; Svenda, Martin; Van der Schot, Gijs; Vartanyants, Ivan A.; Williams, Garth J.; Xavier, P. Lourdu

2017-01-01

Single-particle diffraction from X-ray Free Electron Lasers offers the potential for molecular structure determination without the need for crystallization. In an effort to further develop the technique, we present a dataset of coherent soft X-ray diffraction images of Coliphage PR772 virus, collected at the Atomic Molecular Optics (AMO) beamline with pnCCD detectors in the LAMP instrument at the Linac Coherent Light Source. The diameter of PR772 ranges from 65–70 nm, which is considerably smaller than the previously reported ~600 nm diameter Mimivirus. This reflects continued progress in XFEL-based single-particle imaging towards the single molecular imaging regime. The data set contains significantly more single particle hits than collected in previous experiments, enabling the development of improved statistical analysis, reconstruction algorithms, and quantitative metrics to determine resolution and self-consistency. PMID:28654088

Coherent soft X-ray diffraction imaging of coliphage PR772 at the Linac coherent light source

DOE PAGES

Reddy, Hemanth K. N.; Yoon, Chun Hong; Aquila, Andrew; ...

2017-06-27

Single-particle diffraction from X-ray Free Electron Lasers offers the potential for molecular structure determination without the need for crystallization. In an effort to further develop the technique, we present a dataset of coherent soft X-ray diffraction images of Coliphage PR772 virus, collected at the Atomic Molecular Optics (AMO) beamline with pnCCD detectors in the LAMP instrument at the Linac Coherent Light Source. The diameter of PR772 ranges from 65–70 nm, which is considerably smaller than the previously reported ~600 nm diameter Mimivirus. This reflects continued progress in XFEL-based single-particle imaging towards the single molecular imaging regime. As a result, themore » data set contains significantly more single particle hits than collected in previous experiments, enabling the development of improved statistical analysis, reconstruction algorithms, and quantitative metrics to determine resolution and self-consistency.« less

Coherent soft X-ray diffraction imaging of coliphage PR772 at the Linac coherent light source.

PubMed

Reddy, Hemanth K N; Yoon, Chun Hong; Aquila, Andrew; Awel, Salah; Ayyer, Kartik; Barty, Anton; Berntsen, Peter; Bielecki, Johan; Bobkov, Sergey; Bucher, Maximilian; Carini, Gabriella A; Carron, Sebastian; Chapman, Henry; Daurer, Benedikt; DeMirci, Hasan; Ekeberg, Tomas; Fromme, Petra; Hajdu, Janos; Hanke, Max Felix; Hart, Philip; Hogue, Brenda G; Hosseinizadeh, Ahmad; Kim, Yoonhee; Kirian, Richard A; Kurta, Ruslan P; Larsson, Daniel S D; Duane Loh, N; Maia, Filipe R N C; Mancuso, Adrian P; Mühlig, Kerstin; Munke, Anna; Nam, Daewoong; Nettelblad, Carl; Ourmazd, Abbas; Rose, Max; Schwander, Peter; Seibert, Marvin; Sellberg, Jonas A; Song, Changyong; Spence, John C H; Svenda, Martin; Van der Schot, Gijs; Vartanyants, Ivan A; Williams, Garth J; Xavier, P Lourdu

2017-06-27

Single-particle diffraction from X-ray Free Electron Lasers offers the potential for molecular structure determination without the need for crystallization. In an effort to further develop the technique, we present a dataset of coherent soft X-ray diffraction images of Coliphage PR772 virus, collected at the Atomic Molecular Optics (AMO) beamline with pnCCD detectors in the LAMP instrument at the Linac Coherent Light Source. The diameter of PR772 ranges from 65-70 nm, which is considerably smaller than the previously reported ~600 nm diameter Mimivirus. This reflects continued progress in XFEL-based single-particle imaging towards the single molecular imaging regime. The data set contains significantly more single particle hits than collected in previous experiments, enabling the development of improved statistical analysis, reconstruction algorithms, and quantitative metrics to determine resolution and self-consistency.

Control of ultrafast pulses in a hydrogen-filled hollow-core photonic-crystal fiber by Raman coherence

NASA Astrophysics Data System (ADS)

Belli, F.; Abdolvand, A.; Travers, J. C.; Russell, P. St. J.

2018-01-01

We present the results of an experimental and numerical investigation into temporally nonlocal coherent interactions between ultrashort pulses, mediated by Raman coherence, in a gas-filled kagome-style hollow-core photonic-crystal fiber. A pump pulse first sets up the Raman coherence, creating a refractive index spatiotemporal grating in the gas that travels at the group velocity of the pump pulse. Varying the arrival time of a second, probe, pulse allows a high degree of control over its evolution as it propagates along the fiber through the grating. Of particular interest are soliton-driven effects such as self-compression and dispersive wave (DW) emission. In the experiments reported, a DW is emitted at ˜300 nm and exhibits a wiggling effect, with its central frequency oscillating periodically with pump-probe delay. The results demonstrate that a strong Raman coherence, created in a broadband guiding gas-filled kagome photonic-crystal fiber, can be used to control the nonlinear dynamics of ultrashort probe pulses, even in difficult-to-access spectral regions such as the deep and vacuum ultraviolet.

Highly coherent vacuum ultraviolet radiation at the 15th harmonic with echo-enabled harmonic generation technique

NASA Astrophysics Data System (ADS)

Hemsing, E.; Dunning, M.; Hast, C.; Raubenheimer, T. O.; Weathersby, S.; Xiang, D.

2014-07-01

X-ray free-electron lasers are enabling access to new science by producing ultrafast and intense x rays that give researchers unparalleled power and precision in examining the fundamental nature of matter. In the quest for fully coherent x rays, the echo-enabled harmonic generation technique is one of the most promising methods. In this technique, coherent radiation at the high harmonic frequencies of two seed lasers is generated from the recoherence of electron beam phase space memory. Here we report on the generation of highly coherent and stable vacuum ultraviolet radiation at the 15th harmonic of an infrared seed laser with this technique. The experiment demonstrates two distinct advantages that are intrinsic to the highly nonlinear phase space gymnastics of echo-enabled harmonic generation in a new regime, i.e., high frequency up-conversion efficiency and insensitivity to electron beam phase space imperfections. Our results allow comparison and confirmation of predictive models and scaling laws, and mark a significant step towards fully coherent x-ray free-electron lasers that will open new scientific research.

Soft X-Ray Second Harmonic Generation as an Interfacial Probe

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

Lam, R. K.; Raj, S. L.; Pascal, T. A.

Nonlinear optical processes at soft x-ray wavelengths have remained largely unexplored due to the lack of available light sources with the requisite intensity and coherence. Here we report the observation of soft x-ray second harmonic generation near the carbon K edge (~284 eV) in graphite thin films generated by high intensity, coherent soft x-ray pulses at the FERMI free electron laser. Our experimental results and accompanying first-principles theoretical analysis highlight the effect of resonant enhancement above the carbon K edge and show the technique to be interfacially sensitive in a centrosymmetric sample with second harmonic intensity arising primarily from themore » first atomic layer at the open surface. This technique and the associated theoretical framework demonstrate the ability to selectively probe interfaces, including those that are buried, with elemental specificity, providing a new tool for a range of scientific problems.« less

Soft X-Ray Second Harmonic Generation as an Interfacial Probe

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

Lam, R. K.; Raj, S. L.; Pascal, T. A.

Nonlinear optical processes at soft x-ray wavelengths have remained largely unexplored due to the lack of available light sources with the requisite intensity and coherence. Here we report the observation of soft x-ray second harmonic generation near the carbon K edge (~284 eV) in graphite thin films generated by high intensity, coherent soft x-ray pulses at the FERMI free electron laser. Our experimental results and accompanying first-principles theoretical analysis highlight the effect of resonant enhancement above the carbon K edge and show the technique to be interfacially sensitive in a centrosymmetric sample with second harmonic intensity arising primarily from themore » first atomic layer at the open surface. Here, this technique and the associated theoretical framework demonstrate the ability to selectively probe interfaces, including those that are buried, with elemental specificity, providing a new tool for a range of scientific problems.« less

Soft X-Ray Second Harmonic Generation as an Interfacial Probe

DOE PAGES

Lam, R. K.; Raj, S. L.; Pascal, T. A.; ...

2018-01-08

Nonlinear optical processes at soft x-ray wavelengths have remained largely unexplored due to the lack of available light sources with the requisite intensity and coherence. Here we report the observation of soft x-ray second harmonic generation near the carbon K edge (~284 eV) in graphite thin films generated by high intensity, coherent soft x-ray pulses at the FERMI free electron laser. Our experimental results and accompanying first-principles theoretical analysis highlight the effect of resonant enhancement above the carbon K edge and show the technique to be interfacially sensitive in a centrosymmetric sample with second harmonic intensity arising primarily from themore » first atomic layer at the open surface. Here, this technique and the associated theoretical framework demonstrate the ability to selectively probe interfaces, including those that are buried, with elemental specificity, providing a new tool for a range of scientific problems.« less

Soft X-Ray Second Harmonic Generation as an Interfacial Probe

NASA Astrophysics Data System (ADS)

Lam, R. K.; Raj, S. L.; Pascal, T. A.; Pemmaraju, C. D.; Foglia, L.; Simoncig, A.; Fabris, N.; Miotti, P.; Hull, C. J.; Rizzuto, A. M.; Smith, J. W.; Mincigrucci, R.; Masciovecchio, C.; Gessini, A.; Allaria, E.; De Ninno, G.; Diviacco, B.; Roussel, E.; Spampinati, S.; Penco, G.; Di Mitri, S.; Trovò, M.; Danailov, M.; Christensen, S. T.; Sokaras, D.; Weng, T.-C.; Coreno, M.; Poletto, L.; Drisdell, W. S.; Prendergast, D.; Giannessi, L.; Principi, E.; Nordlund, D.; Saykally, R. J.; Schwartz, C. P.

2018-01-01

Nonlinear optical processes at soft x-ray wavelengths have remained largely unexplored due to the lack of available light sources with the requisite intensity and coherence. Here we report the observation of soft x-ray second harmonic generation near the carbon K edge (˜284 eV ) in graphite thin films generated by high intensity, coherent soft x-ray pulses at the FERMI free electron laser. Our experimental results and accompanying first-principles theoretical analysis highlight the effect of resonant enhancement above the carbon K edge and show the technique to be interfacially sensitive in a centrosymmetric sample with second harmonic intensity arising primarily from the first atomic layer at the open surface. This technique and the associated theoretical framework demonstrate the ability to selectively probe interfaces, including those that are buried, with elemental specificity, providing a new tool for a range of scientific problems.

Single-shot observation of optical rogue waves in integrable turbulence using time microscopy

PubMed Central

Suret, Pierre; Koussaifi, Rebecca El; Tikan, Alexey; Evain, Clément; Randoux, Stéphane; Szwaj, Christophe; Bielawski, Serge

2016-01-01

Optical fibres are favourable tabletop laboratories to investigate both coherent and incoherent nonlinear waves. In particular, exact solutions of the one-dimensional nonlinear Schrödinger equation such as fundamental solitons or solitons on finite background can be generated by launching periodic, specifically designed coherent waves in optical fibres. It is an open fundamental question to know whether these coherent structures can emerge from the nonlinear propagation of random waves. However the typical sub-picosecond timescale prevented—up to now—time-resolved observations of the awaited dynamics. Here, we report temporal ‘snapshots' of random light using a specially designed ‘time-microscope'. Ultrafast structures having peak powers much larger than the average optical power are generated from the propagation of partially coherent waves in optical fibre and are recorded with 250 femtoseconds resolution. Our experiment demonstrates the central role played by ‘breather-like' structures such as the Peregrine soliton in the emergence of heavy-tailed statistics in integrable turbulence. PMID:27713416

Coherent ultrafast spin-dynamics probed in three dimensional topological insulators

PubMed Central

Boschini, F.; Mansurova, M.; Mussler, G.; Kampmeier, J.; Grützmacher, D.; Braun, L.; Katmis, F.; Moodera, J. S.; Dallera, C.; Carpene, E.; Franz, C.; Czerner, M.; Heiliger, C.; Kampfrath, T.; Münzenberg, M.

2015-01-01

Topological insulators are candidates to open up a novel route in spin based electronics. Different to traditional ferromagnetic materials, where the carrier spin-polarization and magnetization are based on the exchange interaction, the spin properties in topological insulators are based on the coupling of spin- and orbit interaction connected to its momentum. Specific ways to control the spin-polarization with light have been demonstrated: the energy momentum landscape of the Dirac cone provides spin-momentum locking of the charge current and its spin. We investigate a spin-related signal present only during the laser excitation studying real and imaginary part of the complex Kerr angle by disentangling spin and lattice contributions. This coherent signal is only present at the time of the pump-pulses’ light field and can be described in terms of a Raman coherence time. The Raman transition involves states at the bottom edge of the conduction band. We demonstrate a coherent femtosecond control of spin-polarization for electronic states at around the Dirac cone. PMID:26510509

Two-dimensional infrared spectroscopy of intermolecular hydrogen bonds in the condensed phase.

PubMed

Elsaesser, Thomas

2009-09-15

Hydrogen bonding plays a key role in the structural, physical, and chemical properties of liquids such as water and in macromolecular structures such as proteins. Vibrational spectroscopy is an important tool for understanding hydrogen bonding because it provides a way to observe local molecular geometries and their interaction with the environment. Linear vibrational spectroscopy has mapped characteristic changes of vibrational spectra and the occurrence of new bands that form upon hydrogen bonding. However, linear vibrational spectroscopy gives very limited insight into ultrafast dynamics of the underlying molecular interactions, such as the motions of hydrogen-bonded groups, energy dissipation and delocalization, and the fluctuations within hydrogen-bonded structures that occur in the ultrafast time domain. Nonlinear vibrational spectroscopy with its femtosecond time resolution can discern these dynamic processes in real time and has emerged as an important tool for unraveling molecular dynamics and for quantifying interactions that govern the vibrational and structural dynamics of hydrogen bonds. This Account reviews recent progress originating from third-order nonlinear methods of coherent multidimensional vibrational spectroscopy. Ultrafast dynamics of intermolecular hydrogen bonds are addressed for a number of prototype systems: hydrogen-bonded carboxylic acid dimers in an aprotic liquid environment, the disordered fluctuating hydrogen-bond network of liquid water, and DNA oligomers interacting with water. Cyclic carboxylic acid dimers display a rich scheme of vibrational couplings, resulting in OH stretching absorption bands with highly complex spectral envelopes. Two-dimensional spectroscopy of acetic acid dimers in a nonpolar liquid environment demonstrates that multiple Fermi resonances of the OH stretching mode with overtones and combination tones of fingerprint vibrations dominate both the 2D and linear absorption spectra. The coupling of the OH stretching mode with low-frequency hydrogen-bonding modes leads to additional progressions and coherent low-frequency hydrogen-bond motions in the subpicosecond time domain. In water, the 2D spectra reveal ultrafast spectral diffusion on a sub-100 fs time scale caused by the ultrafast structural fluctuations of the strongly coupled hydrogen-bond network. Librational motions play a key role for the ultrafast loss of structural memory. Spectral diffusion rates are enhanced by resonant transfer of OH stretching quanta between water molecules, typically occurring on a 100 fs time scale. In DNA oligomers, femtosecond nonlinear vibrational spectroscopy resolves NH and OH stretching bands in the highly congested infrared spectra of these molecules, which contain alternating adenine-thymine pairs. Studies at different levels of hydration reveal the spectral signatures of water molecules directly interacting with the phosphate groups of DNA and of a second water species forming a fluctuating environment around the DNA oligomers. We expect that the application of 2D infrared spectroscopy in an extended spectral range will reveal the intrinsic coupling between water and specific functional units of DNA.

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

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 its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.

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 since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here in this paper, we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.« less

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 since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here in this paper, we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.« less

Breaking resolution limits in ultrafast electron diffraction and microscopy

PubMed Central

Baum, Peter; Zewail, Ahmed H.

2006-01-01

Ultrafast electron microscopy and diffraction are powerful techniques for the study of the time-resolved structures of molecules, materials, and biological systems. Central to these approaches is the use of ultrafast coherent electron packets. The electron pulses typically have an energy of 30 keV for diffraction and 100–200 keV for microscopy, corresponding to speeds of 33–70% of the speed of light. Although the spatial resolution can reach the atomic scale, the temporal resolution is limited by the pulse width and by the difference in group velocities of electrons and the light used to initiate the dynamical change. In this contribution, we introduce the concept of tilted optical pulses into diffraction and imaging techniques and demonstrate the methodology experimentally. These advances allow us to reach limits of time resolution down to regimes of a few femtoseconds and, possibly, attoseconds. With tilted pulses, every part of the sample is excited at precisely the same time as when the electrons arrive at the specimen. Here, this approach is demonstrated for the most unfavorable case of ultrafast crystallography. We also present a method for measuring the duration of electron packets by autocorrelating electron pulses in free space and without streaking, and we discuss the potential of tilting the electron pulses themselves for applications in domains involving nuclear and electron motions. PMID:17056711

Imaging electronic motions by ultrafast electron diffraction

NASA Astrophysics Data System (ADS)

Shao, Hua-Chieh; Starace, Anthony F.

2017-08-01

Recently ultrafast electron diffraction and microscopy have reached unprecedented temporal resolution, and transient structures with atomic precision have been observed in various reactions. It is anticipated that these extraordinary advances will soon allow direct observation of electronic motions during chemical reactions. We therefore performed a series of theoretical investigations and simulations to investigate the imaging of electronic motions in atoms and molecules by ultrafast electron diffraction. Three prototypical electronic motions were considered for hydrogen atoms. For the case of a breathing mode, the electron density expands and contracts periodically, and we show that the time-resolved scattering intensities reflect such changes of the charge radius. For the case of a wiggling mode, the electron oscillates from one side of the nucleus to the other, and we show that the diffraction images exhibit asymmetric angular distributions. The last case is a hybrid mode that involves both breathing and wiggling motions. Owing to the demonstrated ability of ultrafast electrons to image these motions, we have proposed to image a coherent population transfer in lithium atoms using currently available femtosecond electron pulses. A frequency-swept laser pulse adiabatically drives the valence electron of a lithium atom from the 2s to 2p orbitals, and a time-delayed electron pulse maps such motion. Our simulations show that the diffraction images reflect this motion both in the scattering intensities and the angular distributions.

Coherence-domain imaging with harmonic holography

NASA Astrophysics Data System (ADS)

Pu, Ye; Psaltis, Demetri

2017-08-01

Observing the fast dynamics of specific molecules or targets in three-dimensional (3D) space and time inside a crowded and complex environment, such as living cells or tissues, remain one of the grand open challenges in modern science. Harmonic holography tackle this challenge by combining the 3D imaging capability of holography with the ultrafast, coherent optical contrast offered by second-harmonic radiating imaging probes (SHRIMPs). Similar to fluorescence, the second-harmonic signal emitted from SHRIMPs provides a color contrast against the uninterested background scattering, which can be efficiently suppressed by an optical filter. We review the latest developments in SHRIMPs and harmonic holography and discuss their further applications in fluidics and biofluidics.

Coherent electronic wave packet motion in C(60) controlled by the waveform and polarization of few-cycle laser fields.

PubMed

Li, H; Mignolet, B; Wachter, G; Skruszewicz, S; Zherebtsov, S; Süssmann, F; Kessel, A; Trushin, S A; Kling, Nora G; Kübel, M; Ahn, B; Kim, D; Ben-Itzhak, I; Cocke, C L; Fennel, T; Tiggesbäumker, J; Meiwes-Broer, K-H; Lemell, C; Burgdörfer, J; Levine, R D; Remacle, F; Kling, M F

2015-03-27

Strong laser fields can be used to trigger an ultrafast molecular response that involves electronic excitation and ionization dynamics. Here, we report on the experimental control of the spatial localization of the electronic excitation in the C_{60} fullerene exerted by an intense few-cycle (4 fs) pulse at 720 nm. The control is achieved by tailoring the carrier-envelope phase and the polarization of the laser pulse. We find that the maxima and minima of the photoemission-asymmetry parameter along the laser-polarization axis are synchronized with the localization of the coherent electronic wave packet at around the time of ionization.

Full characterization of an attosecond pulse generated using an infrared driver

PubMed Central

Zhang, Chunmei; Brown, Graham G.; Kim, Kyung Taec; Villeneuve, D. M.; Corkum, P. B.

2016-01-01

The physics of attosecond pulse generation requires using infrared driving wavelength to reach the soft X-rays. However, with longer driving wavelength, the harmonic conversion efficiency drops significantly. It makes the conventional attosecond pulse measurement using streaking very difficult due to the low photoionization cross section in the soft X-rays region. In-situ measurement was developed for precisely this purpose. We use in-situ measurement to characterize, in both space and time, an attosecond pulse produced by ultrafast wavefront rotation of a 1.8 μm fundamental beam. We confirm what models suggest – that each beamlet is an isolated attosecond pulse in the time domain. We get almost constant flat wavefront curvature through the whole photon energy range. The measurement method is scalable to the soft X-ray spectral region. PMID:27230961

Real-time 3-D ultrafast ultrasound quasi-static elastography in vivo

PubMed Central

Papadacci, Clement; Bunting, Ethan A.; Konofagou, Elisa E.

2017-01-01

Ultrasound elastography, a technique used to assess mechanical properties of soft tissue is of major interest in the detection of breast cancer as it is stiffer than the surroundings. Techniques such as ultrasound quasi-static elastography have been developed to assess the strain distribution in soft tissues in two dimensions using a quasi-static compression. However, tumors can exhibit very heterogeneous shape, a three dimensions approach would be then necessary to measure accurately the tumor volume and remove operator dependency. To ensure this issue, several 3-D quasi-static elastographic approaches have been proposed. However, all these approaches suffered from a long acquisition time to acquire 3-D volumes resulting in the impossibility to perform real-time and the creation of artifacts. The long acquisition time comes from both the use of focused ultrasound emissions and the fact that the volume was made from a stack of two dimensions images acquired by mechanically translating an ultrasonic array. Being able to acquire volume at high volume rates is thus crucial to perform real-time with a simple freehand compression and to avoid signal decorrelation coming from hand motions or natural motions such as the respiratory. In this study we developed for the first time, the 3-D ultrafast ultrasound quasi-static elastography method to estimate 3-D axial strain distribution in vivo in real-time. Acquisitions were performed with a 2-D matrix array probe of 256 elements (16-by-16 elements). 100 plane waves were emitted at a volume rate of 100 volumes/sec during a continuous motorized compression. 3-D B-mode volumes and 3-D B-mode cumulative axial strain volumes were estimated on a two-layers gelatin phantom with different stiffness, in a stiff inclusion embedded in a soft gelatin phantoms, in a soft inclusion embedded in a stiff gelatin phantom and in an ex vivo canine liver before and after a high focused ultrasound (HIFU) ablation. In each case, we were able to image in real-time and in entire volumes the axial strain distribution and were able to detect the differences between stiff and soft structures with a good sensitivity. In addition, we were able to detect the stiff lesion in the ex vivo canine liver after HIFU ablation. Finally, we demonstrated the in vivo feasibility of the method using freehand compression on the calf of a human volunteer and were able to retrieve 3-D axial strain volume in real-time depicting the differences in stiffness of the two muscles which compose the calf. The 3-D ultrafast ultrasound quasi-static elastography method could have a major clinical impact for the real-time detection in three dimensions of breast cancer in patients using a simple freehand scanning. PMID:27483021

Very high power THz radiation sources

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

Carr, G.L.; Martin, Michael C.; McKinney, Wayne R.

2002-10-31

We report the production of high power (20 watts average, {approx} 1 Megawatt peak) broadband THz light based on coherent emission from relativistic electrons. Such sources are ideal for imaging, for high power damage studies and for studies of non-linear phenomena in this spectral range. We describe the source, presenting theoretical calculations and their experimental verification. For clarity we compare this source to one based on ultrafast laser techniques.

Photoinduced coherent acoustic phonon dynamics inside Mott insulator Sr2IrO4 films observed by femtosecond X-ray pulses

NASA Astrophysics Data System (ADS)

Zhang, Bing-Bing; Liu, Jian; Wei, Xu; Sun, Da-Rui; Jia, Quan-Jie; Li, Yuelin; Tao, Ye

2017-04-01

We investigate the transient photoexcited lattice dynamics in a layered perovskite Mott insulator Sr2IrO4 film by femtosecond X-ray diffraction using a laser plasma-based X-ray source. The ultrafast structural dynamics of Sr2IrO4 thin films are determined by observing the shift and broadening of (0012) Bragg diffraction after excitation by 1.5 eV and 3.0 eV pump photons for films with different thicknesses. The observed transient lattice response can be well interpreted as a distinct three-step dynamics due to the propagation of coherent acoustic phonons generated by photoinduced quasiparticles (QPs). Employing a normalized phonon propagation model, we found that the photoinduced angular shifts of the Bragg peak collapse into a universal curve after introducing normalized coordinates to account for different thicknesses and pump photon energies, pinpointing the origin of the lattice distortion and its early evolution. In addition, a transient photocurrent measurement indicates that the photoinduced QPs are charge neutral excitons. Mapping the phonon propagation and correlating its dynamics with the QP by ultrafast X-ray diffraction (UXRD) establish a powerful way to study electron-phonon coupling and uncover the exotic physics in strongly correlated systems under nonequilibrium conditions.

Lattice-mediated magnetic order melting in TbMnO3

NASA Astrophysics Data System (ADS)

Baldini, Edoardo; Kubacka, Teresa; Mallett, Benjamin P. P.; Ma, Chao; Koohpayeh, Seyed M.; Zhu, Yimei; Bernhard, Christian; Johnson, Steven L.; Carbone, Fabrizio

2018-03-01

Recent ultrafast magnetic-sensitive measurements [Johnson et al., Phys. Rev. B 92, 184429 (2015), 10.1103/PhysRevB.92.184429; Bothschafter et al., Phys. Rev. B 96, 184414 (2017), 10.1103/PhysRevB.96.184414] have revealed a delayed melting of the long-range cycloid spin order in TbMnO3 following photoexcitation across the fundamental Mott-Hubbard gap. The microscopic mechanism behind this slow transfer of energy from the photoexcited carriers to the spin degrees of freedom is still elusive and not understood. Here, we address this problem by combining spectroscopic ellipsometry, ultrafast broadband optical spectroscopy, and ab initio calculations. Upon photoexcitation, we observe the emergence of a complex collective response, which is due to high-energy coherent optical phonons coupled to the out-of-equilibrium charge density. This response precedes the magnetic order melting and is interpreted as the fingerprint of the formation of anti-Jahn-Teller polarons. We propose that the charge localization in a long-lived self-trapped state hinders the emission of magnons and other spin-flip mechanisms, causing the energy transfer from the charge to the spin system to be mediated by the reorganization of the lattice. Furthermore, we provide evidence for the coherent excitation of a phonon mode associated with the ferroelectric phase transition.

Communication: Probing the interaction of infrared antenna arrays and molecular films with ultrafast quantum dynamics

NASA Astrophysics Data System (ADS)

Cohn, Bar; Prasad, Amit K.; Chuntonov, Lev

2018-04-01

Narrowband vibrational molecular transitions interacting with the broadband resonance of infrared plasmonic antennas lead to Fano lineshapes observed in linear (FTIR) and third-order (transient absorption and 2DIR) spectroscopic experiments. Both molecular and plasmonic components are inherently dissipative, and the effects associated with their coupling can be observed, in principle, when measuring the corresponding ultrafast quantum dynamics. We used 2DIR spectroscopy to study the waiting time evolution of quantum coherence excited in the carbonyl stretching modes of rhodium (acetylacetonato) dicarbonyl molecules, which were embedded in an 80 nm-thick polymer film spin-coated on an array of infrared half-wavelength gold antennas. Despite the pronounced Fano lineshapes obtained for the molecular transitions, and up to a four order of magnitude enhancement of the third-order signals, which taken together, indicate the coupling between the plasmonic and molecular transitions, the dynamics of the quantum coherence were identical to that obtained with 3 μm-thick film without the interaction with the plamson mode. This suggests that the coupling rate between the molecular and plasmonic excitations is significantly smaller than the relaxation rates of the molecular excitations monitored in the experiment. Here, the Fano lineshape, observed at the frequency of the molecular transition, can result from the mutual radiation damping of the molecular and plasmon modes.

High-speed optical coherence tomography by circular interferometric ranging

NASA Astrophysics Data System (ADS)

Siddiqui, Meena; Nam, Ahhyun S.; Tozburun, Serhat; Lippok, Norman; Blatter, Cedric; Vakoc, Benjamin J.

2018-02-01

Existing three-dimensional optical imaging methods excel in controlled environments, but are difficult to deploy over large, irregular and dynamic fields. This means that they can be ill-suited for use in areas such as material inspection and medicine. To better address these applications, we developed methods in optical coherence tomography to efficiently interrogate sparse scattering fields, that is, those in which most locations (voxels) do not generate meaningful signal. Frequency comb sources are used to superimpose reflected signals from equispaced locations through optical subsampling. This results in circular ranging, and reduces the number of measurements required to interrogate large volumetric fields. As a result, signal acquisition barriers that have limited speed and field in optical coherence tomography are avoided. With a new ultrafast, time-stretched frequency comb laser design operating with 7.6 MHz to 18.9 MHz repetition rates, we achieved imaging of multi-cm3 fields at up to 7.5 volumes per second.

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.

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.

Large optical nonlinearity of indium tin oxide in its epsilon-near-zero region.

PubMed

Alam, M Zahirul; De Leon, Israel; Boyd, Robert W

2016-05-13

Nonlinear optical phenomena are crucial for a broad range of applications, such as microscopy, all-optical data processing, and quantum information. However, materials usually exhibit a weak optical nonlinearity even under intense coherent illumination. We report that indium tin oxide can acquire an ultrafast and large intensity-dependent refractive index in the region of the spectrum where the real part of its permittivity vanishes. We observe a change in the real part of the refractive index of 0.72 ± 0.025, corresponding to 170% of the linear refractive index. This change in refractive index is reversible with a recovery time of about 360 femtoseconds. Our results offer the possibility of designing material structures with large ultrafast nonlinearity for applications in nanophotonics. Copyright © 2016, American Association for the Advancement of Science.

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

DOE PAGES

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

2015-04-02

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

Feasibility study of generating ultra-high harmonic radiation with a single stage echo-enabled harmonic generation scheme

NASA Astrophysics Data System (ADS)

Zhou, Kaishang; Feng, Chao; Wang, Dong

2016-10-01

The echo enabled harmonic generation (EEHG) scheme holds the ability for the generation of fully coherent soft x-ray free-electron laser (FEL) pulses directly from external UV seeding sources. In this paper, we study the feasibility of using a single stage EEHG to generate coherent radiation in the "water window" and beyond. Using the high-order operating modes of the EEHG scheme, intensive numerical simulations have been performed considering various three-dimensional effects. The simulation results demonstrated that coherent soft x-ray radiation at 150th harmonic (1.77 nm) of the seed can be produced by a single stage EEHG. The decreasing of the final bunching factor at the desired harmonic caused by intra beam scattering (IBS) effect has also been analyzed.

Application of Soft Computing in Coherent Communications Phase Synchronization

NASA Technical Reports Server (NTRS)

Drake, Jeffrey T.; Prasad, Nadipuram R.

2000-01-01

The use of soft computing techniques in coherent communications phase synchronization provides an alternative to analytical or hard computing methods. This paper discusses a novel use of Adaptive Neuro-Fuzzy Inference Systems (ANFIS) for phase synchronization in coherent communications systems utilizing Multiple Phase Shift Keying (MPSK) modulation. A brief overview of the M-PSK digital communications bandpass modulation technique is presented and it's requisite need for phase synchronization is discussed. We briefly describe the hybrid platform developed by Jang that incorporates fuzzy/neural structures namely the, Adaptive Neuro-Fuzzy Interference Systems (ANFIS). We then discuss application of ANFIS to phase estimation for M-PSK. The modeling of both explicit, and implicit phase estimation schemes for M-PSK symbols with unknown structure are discussed. Performance results from simulation of the above scheme is presented.

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 of transient, excited states, providing quantification of important parameters such as spin and orbital angular momenta as well as the energy gaps that separate electronic fine structure states. Ultrafast two-dimensional electronic spectroscopy (2DES) can be used to understand how these details influence state-to-state carrier dynamics. In combination, VTVH and 2DES methods can provide chemists with detailed information regarding the structure-dependent and state-specific flow of energy through metal nanoclusters. In this Account, we highlight recent advances toward understanding structure-dependent carrier dynamics for metals spanning the sub-nanometer to tens of nanometers length scale. We demonstrate the use of UCLEM methods for arresting interband scattering effects. For sub-nanometer thiol-protected nanoclusters, we discuss the effectiveness of VTVH for distinguishing state-specific radiative recombination originating from a gold core versus organometallic protecting layers. This state specificity is refined further using femtosecond 2DES and two-color methods to isolate so-called superatom state dynamics and vibrationally mediated spin-conversion and emission processes. Finally, we discuss prospects for merging VTVH and 2DES methods into a single platform.

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.

Characteristics of soft x-ray spectra from ultra-fast micro-capillary discharge plasmas

NASA Astrophysics Data System (ADS)

Li, Jing; Avaria, Gonzalo; Shlyaptsev, Vyacheslav; Tomasel, Fernando; Grisham, Michael; Dawson, Quincy; Rocca, Jorge; NSF CenterExtreme Ultraviolet Science; Technology Collaboration

2013-10-01

The efficient generation of high aspect ratio (e.g. 300:1) plasma columns ionized to very high degrees of ionization (e.g. Ni-like Xenon) by an ultrafast current pulses of moderate amplitude in micro-capillary channels is of interest for fundamental plasma studies and for applications such as the generation of discharge-pumped soft x-ray lasers. Spectra and simulations for plasmas generated in 500 um alumina capillary discharges driven by 35-40 kA current pulses with 4 ns rise time were obtained in Xenon and Neon discharges. The first shows the presence of lines corresponding to ionization stages up to Fe-like Xe. The latter show that Al impurities from the walls and Si (from injected SiH4) are ionized to the H-like and He-like stages. He-like spectra containing the resonance line significantly broaden by opacity, the intercombination line, and Li-like satellites are analyzed and modeled. For Xenon discharges, the spectral lines from the Ni-like transitions the 3d94d(3/2, 3/2)J=0 to the 3d94p(5/2, 3/2)J=1 and to 3d94p(3/2, 1/2)J=1 are observed at gas pressures up to 2.0 Torr. Work supported by NSF Award PHY-1004295.

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

NASA Astrophysics Data System (ADS)

Dlott, Dana

2008-03-01

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

Femtosecond Optics: Advanced Devices and Ultrafast Phenomena

DTIC Science & Technology

2007-05-31

repetition rate from a soliton fiber laser [6]. Because the mode- locking mechanism is passive, no external oscillator is required, leading to a more...nonlinearity, 1.8 m of LNL-SMF is included in the laser. Mode- locked operation of the laser was obtained through nonlinear polarization evolution [6]. For pump...Generation in Photonic Crystal Fibers for Optical Coherence Tomography H. Frequency Swept Lasers and Fourier Domain Mode Locking (FDML) I. Physics of

Complete Quantum Control of a Single Silicon-Vacancy Center in a Diamond Nanopillar

NASA Astrophysics Data System (ADS)

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan-Kai; Dory, Constantin; Radulaski, Marina; Kelaita, Yousif; Shen, Zhi-Xun; Melosh, Nicholas A.; Chu, Steven; Vuckovic, Jelena

Coherent quantum control of a quantum bit (qubit) is an important step towards its use in a quantum network. SiV- center in diamond offers excellent physical qualities such as low inhomogeneous broadening, fast photon emission, and a large Debye-Waller factor, while the fast spin manipulation and techniques to extend the spin coherence time are under active investigation. Here, we demonstrate full coherent control over the state of a single SiV- center in a diamond nanopillar using ultrafast optical pulses. The high quality of the chemical vapor deposition grown SiV- centers allows us to coherently manipulate and quasi-resonantly read out the state of the single SiV- center. Moreover, the SiV- centers being coherently controlled are integrated into diamond nanopillar arrays in a site-controlled, individually addressable manner with high yield, low strain, and high spectral stability, which paves the way for scalable on chip optically accessible quantum system in a quantum photonic network. Financial support is provided by the DOE Office of Basic Energy Sciences, Division of Materials Sciences through Stanford Institute for Materials and Energy Sciences (SIMES) under contract DE-AC02-76SF00515.

0.5-keV Soft X-ray attosecond continua

PubMed Central

Teichmann, S. M.; Silva, F.; Cousin, S. L.; Hemmer, M.; Biegert, J.

2016-01-01

Attosecond light pulses in the extreme ultraviolet have drawn a great deal of attention due to their ability to interrogate electronic dynamics in real time. Nevertheless, to follow charge dynamics and excitations in materials, element selectivity is a prerequisite, which demands such pulses in the soft X-ray region, above 200 eV, to simultaneously cover several fundamental absorption edges of the constituents of the materials. Here, we experimentally demonstrate the exploitation of a transient phase matching regime to generate carrier envelope controlled soft X-ray supercontinua with pulse energies up to 2.9±0.1 pJ and a flux of (7.3±0.1) × 107 photons per second across the entire water window and attosecond pulses with 13 as transform limit. Our results herald attosecond science at the fundamental absorption edges of matter by bridging the gap between ultrafast temporal resolution and element specific probing. PMID:27167525

Coherent control of ultrafast optical four-wave mixing with two-color {omega}-3{omega} laser pulses

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

Serrat, Carles

2005-08-15

A theoretical investigation on the coherent control of optical transient four-wave mixing interactions in two-level systems with two intense few-cycle propagating laser pulses of central angular frequencies {omega} and 3{omega} is reported. By numerically solving the full Maxwell-Bloch equations beyond the slowly varying envelope and rotating-wave approximations in the time domain, the nonlinear coupling to the optical field at frequency 5{omega} is found to depend critically on the initial relative phase {phi} of the propagating pulses: the coupling is enhanced when the pulses interfere constructively in the center ({phi}=0), while it is nearly suppressed when they are out of phasemore » ({phi}={pi})« less

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

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

NASA Astrophysics Data System (ADS)

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

2015-09-01

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

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.

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.

Coherent generation of symmetry-forbidden phonons by light-induced electron-phonon interactions in magnetite

NASA Astrophysics Data System (ADS)

Borroni, S.; Baldini, E.; Katukuri, V. M.; Mann, A.; Parlinski, K.; Legut, D.; Arrell, C.; van Mourik, F.; Teyssier, J.; Kozlowski, A.; Piekarz, P.; Yazyev, O. V.; Oleś, A. M.; Lorenzana, J.; Carbone, F.

2017-09-01

Symmetry breaking across phase transitions often causes changes in selection rules and emergence of optical modes which can be detected via spectroscopic techniques or generated coherently in pump-probe experiments. In second-order or weakly first-order transitions, fluctuations of the ordering field are present above the ordering temperature, giving rise to intriguing precursor phenomena, such as critical opalescence. Here, we demonstrate that in magnetite (Fe3O4 ) light excitation couples to the critical fluctuations of the charge order and coherently generates structural modes of the ordered phase above the critical temperature of the Verwey transition. Our findings are obtained by detecting coherent oscillations of the optical constants through ultrafast broadband spectroscopy and analyzing their dependence on temperature. To unveil the coupling between the structural modes and the electronic excitations, at the origin of the Verwey transition, we combine our results from pump-probe experiments with spontaneous Raman scattering data and theoretical calculations of both the phonon dispersion curves and the optical constants. Our methodology represents an effective tool to study the real-time dynamics of critical fluctuations across phase transitions.

Communication: Coherences observed in vivo in photosynthetic bacteria using two-dimensional electronic spectroscopy

NASA Astrophysics Data System (ADS)

Dahlberg, Peter D.; Norris, Graham J.; Wang, Cheng; Viswanathan, Subha; Singh, Ved P.; Engel, Gregory S.

2015-09-01

Energy transfer through large disordered antenna networks in photosynthetic organisms can occur with a quantum efficiency of nearly 100%. This energy transfer is facilitated by the electronic structure of the photosynthetic antennae as well as interactions between electronic states and the surrounding environment. Coherences in time-domain spectroscopy provide a fine probe of how a system interacts with its surroundings. In two-dimensional electronic spectroscopy, coherences can appear on both the ground and excited state surfaces revealing detailed information regarding electronic structure, system-bath coupling, energy transfer, and energetic coupling in complex chemical systems. Numerous studies have revealed coherences in isolated photosynthetic pigment-protein complexes, but these coherences have not been observed in vivo due to the small amplitude of these signals and the intense scatter from whole cells. Here, we present data acquired using ultrafast video-acquisition gradient-assisted photon echo spectroscopy to observe quantum beating signals from coherences in vivo. Experiments were conducted on isolated light harvesting complex II (LH2) from Rhodobacter sphaeroides, whole cells of R. sphaeroides, and whole cells of R. sphaeroides grown in 30% deuterated media. A vibronic coherence was observed following laser excitation at ambient temperature between the B850 and the B850∗ states of LH2 in each of the 3 samples with a lifetime of ˜40-60 fs.

Optical subcarrier processing for Nyquist SCM signals via coherent spectrum overlapping in four-wave mixing with coherent multi-tone pump.

PubMed

Lu, Guo-Wei; Luís, Ruben S; Mendinueta, José Manuel Delgado; Sakamoto, Takahide; Yamamoto, Naokatsu

2018-01-22

As one of the promising multiplexing and multicarrier modulation technologies, Nyquist subcarrier multiplexing (Nyquist SCM) has recently attracted research attention to realize ultra-fast and ultra-spectral-efficient optical networks. In this paper, we propose and experimentally demonstrate optical subcarrier processing technologies for Nyquist SCM signals such as frequency conversion, multicast and data aggregation of subcarriers, through the coherent spectrum overlapping between subcarriers in four-wave mixing (FWM) with coherent multi-tone pump. The data aggregation is realized by coherently superposing or combining low-level subcarriers to yield high-level subcarriers in the optical field. Moreover, multiple replicas of the data-aggregated subcarriers and the subcarriers carrying the original data are obtained. In the experiment, two 5 Gbps quadrature phase-shift keying (QPSK) subcarriers are coherently combined to generate a 10 Gbps 16 quadrature amplitude modulation (QAM) subcarrier with frequency conversions through the FWM with coherent multi-tone pump. Less than 1 dB optical signal-to-noise ratio (OSNR) penalty variation is observed for the synthesized 16QAM subcarriers after the data aggregation. In addition, some subcarriers are kept in the original formats, QPSK, with a power penalty of less than 0.4 dB with respect to the original input subcarriers. The proposed subcarrier processing technology enables flexibility for spectral management in future dynamic optical networks.

A new coupling mechanism between two graphene electron waveguides for ultrafast switching

NASA Astrophysics Data System (ADS)

Huang, Wei; Liang, Shi-Jun; Kyoseva, Elica; Ang, Lay Kee

2018-03-01

In this paper, we report a novel coupling between two graphene electron waveguides, in analogy the optical waveguides. The design is based on the coherent quantum mechanical tunneling of Rabi oscillation between the two graphene electron waveguides. Based on this coupling mechanism, we propose that it can be used as an ultrafast electronic switching device. Based on a modified coupled mode theory, we construct a theoretical model to analyze the device characteristics, and predict that the switching speed is faster than 1 ps and the on-off ratio exceeds 106. Due to the long mean free path of electrons in graphene at room temperature, the proposed design avoids the limitation of low temperature operation required in the traditional design by using semiconductor quantum-well structure. The layout of our design is similar to that of a standard complementary metal-oxide-semiconductor transistor that should be readily fabricated with current state-of-art nanotechnology.

Generation of coherent terahertz radiation in ultrafast laser-gas interactionsa)

NASA Astrophysics Data System (ADS)

Kim, Ki-Yong

2009-05-01

The generation of intense terahertz radiation in ultrafast laser-gas interactions is studied on a basis of transient electron current model. When an ultrashort pulse laser's fundamental and its second harmonic fields are mixed to ionize a gas, a nonvanishing, directional photoelectron current can be produced, which simultaneously emits terahertz radiation in the far field. Here, the generation mechanism is examined with an analytic derivation and numerical simulations, in which tunneling ionization and subsequent electron motion in the combined laser field play a key role. In the simulations, three types of laser-gas interactions are considered: (i) mixing the fundamental and its second harmonic fields, (ii) mixing nonharmonic, two-color fields, and (iii) focusing single-color, few-cycle pulses. In these interactions, terahertz generation and other nonlinear effects driven by the transient current are investigated. In particular, anticorrelation between terahertz and second (or third) harmonic generation is observed and analyzed.

Femtosecond X-ray Fourier holography imaging of free-flying nanoparticles

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

Gorkhover, Tais; Ulmer, Anatoli; Ferguson, Ken

Ultrafast X-ray imaging on individual fragile specimens such as aerosols, metastable particles, superfluid quantum systems and live biospecimens provides high-resolution information that is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imaging, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely defined. Here in this paper, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highest lateral resolutionmore » so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond timescale.« less

Femtosecond X-ray Fourier holography imaging of free-flying nanoparticles

NASA Astrophysics Data System (ADS)

Gorkhover, Tais; Ulmer, Anatoli; Ferguson, Ken; Bucher, Max; Maia, Filipe R. N. C.; Bielecki, Johan; Ekeberg, Tomas; Hantke, Max F.; Daurer, Benedikt J.; Nettelblad, Carl; Andreasson, Jakob; Barty, Anton; Bruza, Petr; Carron, Sebastian; Hasse, Dirk; Krzywinski, Jacek; Larsson, Daniel S. D.; Morgan, Andrew; Mühlig, Kerstin; Müller, Maria; Okamoto, Kenta; Pietrini, Alberto; Rupp, Daniela; Sauppe, Mario; van der Schot, Gijs; Seibert, Marvin; Sellberg, Jonas A.; Svenda, Martin; Swiggers, Michelle; Timneanu, Nicusor; Westphal, Daniel; Williams, Garth; Zani, Alessandro; Chapman, Henry N.; Faigel, Gyula; Möller, Thomas; Hajdu, Janos; Bostedt, Christoph

2018-03-01

Ultrafast X-ray imaging on individual fragile specimens such as aerosols1, metastable particles2, superfluid quantum systems3 and live biospecimens4 provides high-resolution information that is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imaging, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely defined4,5. Here, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highest lateral resolution so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond timescale.

Compression of high-density 0.16 pC electron bunches through high field gradients for ultrafast single shot electron diffraction: The Compact RF Gun

PubMed Central

Daoud, Hazem; Floettmann, Klaus; Dwayne Miller, R. J.

2017-01-01

We present an RF gun design for single shot ultrafast electron diffraction experiments that can produce sub-100 fs high-charge electron bunches in the 130 keV energy range. Our simulations show that our proposed half-cell RF cavity is capable of producing 137 keV, 27 fs rms (60 fs FWHM), 106 electron bunches with an rms spot size of 276 μm and a transverse coherence length of 2.0 nm. The required operation power is 9.2 kW, significantly lower than conventional rf cavity designs and a key design feature. This electron source further relies on high electric field gradients at the cathode to simultaneously accelerate and compress the electron bunch to open up new space-time resolution domains for atomically resolved dynamics. PMID:28428973

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

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

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

PubMed

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

2018-05-02

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

Understanding the features in the ultrafast transient absorption spectra of CdSe quantum dots

NASA Astrophysics Data System (ADS)

Zhang, Cheng; Do, Thanh Nhut; Ong, Xuanwei; Chan, Yinthai; Tan, Howe-Siang

2016-12-01

We describe a model to explain the features of the ultrafast transient absorption (TA) spectra of CdSe core type quantum dots (QDs). The measured TA spectrum consists of contributions by the ground state bleach (GSB), stimulated emission (SE) and excited state absorption (ESA) processes associated with the three lowest energy transition of the QDs. We model the shapes of the GSB, SE and ESA spectral components after fits to the linear absorption. The spectral positions of the ESA components take into account the biexcitonic binding energy. In order to obtain the correct weightage of the GSB, SE and ESA components to the TA spectrum, we enumerate the set of coherence transfer pathways associated with these processes. From our fits of the experimental TA spectra of 65 Å diameter QDs, biexcitonic binding energies for the three lowest energy transitions are obtained.

Femtosecond X-ray Fourier holography imaging of free-flying nanoparticles

DOE PAGES

Gorkhover, Tais; Ulmer, Anatoli; Ferguson, Ken; ...

2018-02-26

Ultrafast X-ray imaging on individual fragile specimens such as aerosols, metastable particles, superfluid quantum systems and live biospecimens provides high-resolution information that is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imaging, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely defined. Here in this paper, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highest lateral resolutionmore » so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond timescale.« less

2010 MULTIPHOTON PROCESSES GORDON RESEARCH CONFERENCE, JUNE 6-11, 2010, TILTON, NH

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

Mette Gaarde

2010-06-11

The Gordon Research Conference on Multiphoton Processes will be held for the 15th time in 2010. The meeting continues to evolve as it embraces both the rapid technological and intellectual growth in the field as well as the multi-disciplinary expertise of the participants. This time the sessions will focus on: (1) Ultrafast coherent control; (2) Free-electron laser experiments and theory; (3) Generation of harmonics and attosecond pulses; (4) Ultrafast imaging; (5) Applications of very high intensity laser fields; (6) Strong-field processes in molecules and solids; (7) Attosecond science; and (8) Controlling light. The scientific program will blur traditional disciplinary boundariesmore » as the presenters and discussion leaders involve chemists, physicists, and optical engineers, representing both experiment and theory. The broad range of expertise and different perspectives of attendees should provide a stimulating and unique environment for solving problems and developing new ideas in this rapidly evolving field.« less

Mapping carrier diffusion in single silicon core-shell nanowires with ultrafast optical microscopy.

PubMed

Seo, M A; Yoo, J; Dayeh, S A; Picraux, S T; Taylor, A J; Prasankumar, R P

2012-12-12

Recent success in the fabrication of axial and radial core-shell heterostructures, composed of one or more layers with different properties, on semiconductor nanowires (NWs) has enabled greater control of NW-based device operation for various applications. (1-3) However, further progress toward significant performance enhancements in a given application is hindered by the limited knowledge of carrier dynamics in these structures. In particular, the strong influence of interfaces between different layers in NWs on transport makes it especially important to understand carrier dynamics in these quasi-one-dimensional systems. Here, we use ultrafast optical microscopy (4) to directly examine carrier relaxation and diffusion in single silicon core-only and Si/SiO(2) core-shell NWs with high temporal and spatial resolution in a noncontact manner. This enables us to reveal strong coherent phonon oscillations and experimentally map electron and hole diffusion currents in individual semiconductor NWs for the first time.

High peak power THz source for ultrafast electron diffraction

NASA Astrophysics Data System (ADS)

Liu, Shengguang

2018-01-01

Terahertz (THz) science and technology have already become the research highlight at present. In this paper, we put forward a device setup to carry out ultrafast fundamental research. A photocathode RF gun generates electron bunches with ˜MeV energy, ˜ps bunch width and about 25pC charge. The electron bunches inject the designed wiggler, the coherent radiation at THz spectrum emits from these bunches and increases rapidly until the saturation at ˜MW within a short wiggler. THz pulses can be used as pump to stimulate an ultra-short excitation in some kind of sample. Those electron bunches out of wiggler can be handled into bunches with ˜1pC change, small beam spot and energy spread to be probe. Because the pump and probe comes from the same electron source, synchronization between pump and probe is inherent. The whole facility can be compacted on a tabletop.

Electron heating and thermal relaxation of gold nanorods revealed by two-dimensional electronic spectroscopy.

PubMed

Lietard, Aude; Hsieh, Cho-Shuen; Rhee, Hanju; Cho, Minhaeng

2018-03-01

To elucidate the complex interplay between the size and shape of gold nanorods and their electronic, photothermal, and optical properties for molecular imaging, photothermal therapy, and optoelectronic devices, it is a prerequisite to characterize ultrafast electron dynamics in gold nanorods. Time-resolved transient absorption (TA) studies of plasmonic electrons in various nanostructures have revealed the time scales for electron heating, lattice vibrational excitation, and phonon relaxation processes in condensed phases. However, because linear spectroscopic and time-resolved TA signals are vulnerable to inhomogeneous line-broadening, pure dephasing and direct electron heating effects are difficult to observe. Here we show that femtosecond two-dimensional electronic spectroscopy, with its unprecedented time resolution and phase sensitivity, can be used to collect direct experimental evidence for ultrafast electron heating, anomalously strong coherent and transient electronic plasmonic responses, and homogenous dephasing processes resulting from electron-vibration couplings even for polydisperse gold nanorods.

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

DOE PAGES

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

2017-08-31

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

Hybrid Photon-Plasmon Coupling and Ultrafast Control of Nanoantennas on a Silicon Photonic Chip.

PubMed

Chen, Bigeng; Bruck, Roman; Traviss, Daniel; Khokhar, Ali Z; Reynolds, Scott; Thomson, David J; Mashanovich, Goran Z; Reed, Graham T; Muskens, Otto L

2018-01-10

Hybrid integration of nanoplasmonic devices with silicon photonic circuits holds promise for a range of applications in on-chip sensing, field-enhanced and nonlinear spectroscopy, and integrated nanophotonic switches. Here, we demonstrate a new regime of photon-plasmon coupling by combining a silicon photonic resonator with plasmonic nanoantennas. Using principles from coherent perfect absorption, we make use of standing-wave light fields to maximize the photon-plasmon interaction strength. Precise placement of the broadband antennas with respect to the narrowband photonic racetrack modes results in controlled hybridization of only a subset of these modes. By combining antennas into groups of radiating dipoles with opposite phase, far-field scattering is effectively suppressed. We achieve ultrafast tuning of photon-plasmon hybridization including reconfigurable routing of the standing-wave input between two output ports. Hybrid photonic-plasmonic resonators provide conceptually new approaches for on-chip integrated nanophotonic devices.

Combining THz laser excitation with resonant soft X-ray scattering at the Linac Coherent Light Source

DOE PAGES

Turner, Joshua J.; Dakovski, Georgi L.; Hoffmann, Matthias C.; ...

2015-04-11

This paper describes the development of new instrumentation at the Linac Coherent Light Source for conducting THz excitation experiments in an ultra high vacuum environment probed by soft X-ray diffraction. This consists of a cantilevered, fully motorized mirror system which can provide 600 kV cm⁻¹ electric field strengths across the sample and an X-ray detector that can span the full Ewald sphere with in-vacuum motion. The scientific applications motivated by this development, the details of the instrument, and spectra demonstrating the field strengths achieved using this newly developed system are discussed.

Revealing the ultrafast outflow in IRAS 13224-3809 through spectral variability

NASA Astrophysics Data System (ADS)

Parker, M. L.; Alston, W. N.; Buisson, D. J. K.; Fabian, A. C.; Jiang, J.; Kara, E.; Lohfink, A.; Pinto, C.; Reynolds, C. S.

2017-08-01

We present an analysis of the long-term X-ray variability of the extreme narrow-line Seyfert 1 galaxy IRAS 13224-3809 using principal component analysis (PCA) and fractional excess variability (Fvar) spectra to identify model-independent spectral components. We identify a series of variability peaks in both the first PCA component and Fvar spectrum which correspond to the strongest predicted absorption lines from the ultrafast outflow (UFO) discovered by Parker et al. (2017). We also find higher order PCA components, which correspond to variability of the soft excess and reflection features. The subtle differences between RMS and PCA results argue that the observed flux-dependence of the absorption is due to increased ionization of the gas, rather than changes in column density or covering fraction. This result demonstrates that we can detect outflows from variability alone and that variability studies of UFOs are an extremely promising avenue for future research.

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 far-infrared studies of vanadates &mdash Multiple routes for an insulator to metal transition

NASA Astrophysics Data System (ADS)

Liu, Mengkun

The metal insulator transition in vanadates has been studied for decades and yet new discoveries still spring up revealing new physics, especially among two of the most studied members: Vanadium sesquioxide (V20 3) and Vanadium dioxide (VO2). Although subtleties abound, both of the materials have first order insulator to metal phase transitions that are considered to be related to strong electron-electron (e-e) correlation. Further, ultrafast spectroscopy of strongly correlated materials has generated great interest in the field given the potential to dynamically distinguish the difference between electronic (spin) response versus lattice responses due to the associated characteristic energy and time scales. In this thesis, I mainly focus on utilizing ultrafast optical and THz spectroscopy to study phase transition dynamics in high quality V20 3 and VO2 thin films epitaxially grown on different substrates. The main findings of the thesis are: (1) Despite the fact that the insulator to metal transition (IMT) in V203 is electron-correlation driven, lattice distortion plays an important role. Coherent oscillations in the far-infrared conductivity are observed resulting from coherent acoustic phonon modulation of the bandwidth W. The same order of lattice distortion induces less of an effect on the electron transport in VO2 in comparison to V203. This is directly related to the difference in latent heat of the phase transitions in VO2 and V203. (2) It is possible for the IMT to occur with very little structural change in epitaxial strained VO2 films, like in the case of Cr doped or strained V203. However, in V02, this necessitates a large strain which is only possible by clamping to a substrate with larger c axis parameter through epitaxial growth. This is demonstrated for VO 2 films on TiO2 substrates. (3) Initiating an ultrafast photo-induced insulator-to-metal transition (IMT) is not only possible with above bandgap excitation, but also possible with high-field far-infrared excitation. With the help of the field enhancement in metamaterial split ring resonator gaps, we obtain picosecond THz electric field transients of several MV/cm which is sufficient to drive the insulator to metal transition in V02.

Low-Frequency Coherence Break in the Soft X-Ray State of GRS 1915+105

NASA Technical Reports Server (NTRS)

Ji, Jian-Feng; Zhang, Shuang-nan; Qu, Jin-Lu; Li, Ti-Pei

2003-01-01

We present results from the analysis of X-ray power density spectra and coherence when GRS 1915+105 is in soft states. We use three data sets that belong to mu, phi, and delta classes as found in the work of Belloni et al. We find that the power density spectra appear t o be complex, with several features between 0.01 and 10 Hz. The coherence deviates from unity above a characteristic frequency. We discuss our results from different models. The corona size in the sphere-disk model implied by this break frequency is on the order of 10(exp 4) GM/c(exp 2), which is unphysical. Our results are more consistent with the prediction of the model of a planar corona sustained by magnetic flares, in which the characteristic frequency is associated with the longest timescale of an individual flare, which is about 8 s.

PREFACE: Ultrafast and nonlinear optics in carbon nanomaterials

NASA Astrophysics Data System (ADS)

Kono, Junichiro

2013-02-01

Carbon-based nanomaterials—single-wall carbon nanotubes (SWCNTs) and graphene, in particular—have emerged in the last decade as novel low-dimensional systems with extraordinary properties. Because they are direct-bandgap systems, SWCNTs are one of the leading candidates to unify electronic and optical functions in nanoscale circuitry; their diameter-dependent bandgaps can be utilized for multi-wavelength devices. Graphene's ultrahigh carrier mobilities are promising for high-frequency electronic devices, while, at the same time, it is predicted to have ideal properties for terahertz generation and detection due to its unique zero-gap, zero-mass band structure. There have been a large number of basic optical studies on these materials, but most of them were performed in the weak-excitation, quasi-equilibrium regime. In order to probe and assess their performance characteristics as optoelectronic materials under device-operating conditions, it is crucial to strongly drive them and examine their optical properties in highly non-equilibrium situations and with ultrashot time resolution. In this section, the reader will find the latest results in this rapidly growing field of research. We have assembled contributions from some of the leading experts in ultrafast and nonlinear optical spectroscopy of carbon-based nanomaterials. Specific topics featured include: thermalization, cooling, and recombination dynamics of photo-generated carriers; stimulated emission, gain, and amplification; ultrafast photoluminescence; coherent phonon dynamics; exciton-phonon and exciton-plasmon interactions; exciton-exciton annihilation and Auger processes; spontaneous and stimulated emission of terahertz radiation; four-wave mixing and harmonic generation; ultrafast photocurrents; the AC Stark and Franz-Keldysh effects; and non-perturbative light-mater coupling. We would like to express our sincere thanks to those who contributed their latest results to this special section, and the Journal of Physics: Condensed Matter staff for their help, patience and professionalism. Since this is a fast-moving field, there is absolutely no way of presenting definitive answers to all open questions, but we hope that this special section will provide an overview of the current state of knowledge regarding this topic. Furthermore, we hope that the exciting science and technology described in this section will attract and inspire other researchers and students working in related fields to enter into the study of ultrafast and nonlinear optical phenomena in carbon-based nanostructures. Ultrafast and nonlinear optics in carbon nanomaterials contents Ultrafast and nonlinear optics in carbon nanomaterialsJunichiro Kono The impact of pump fluence on carrier relaxation dynamics in optically excited grapheneT Winzer and E Malic Time-resolved spectroscopy on epitaxial graphene in the infrared spectral range: relaxation dynamics and saturation behaviorS Winnerl, F Göttfert, M Mittendorff, H Schneider, M Helm, T Winzer, E Malic, A Knorr, M Orlita, M Potemski, M Sprinkle, C Berger and W A de Heer Nonlinear optics of graphene in a strong magnetic fieldXianghan Yao and Alexey Belyanin Theory of coherent phonons in carbon nanotubes and graphene nanoribbonsG D Sanders, A R T Nugraha, K Sato, J-H Kim3, J Kono3, R Saito and C J Stanton Non-perturbative effects of laser illumination on the electrical properties of graphene nanoribbons Hernán L Calvo, Pablo M Perez-Piskunow, Horacio M Pastawski, Stephan Roche and Luis E F Foa Torres Transient absorption microscopy studies of energy relaxation in graphene oxide thin film Sean Murphy and Libai Huang Femtosecond dynamics of exciton localization: self-trapping from the small to the large polaron limit F X Morrissey, J G Mance, A D Van Pelt and S L Dexheimer

Towards Single-Shot Detection of Bacterial Endospores via Coherent Raman Spectroscopy

NASA Astrophysics Data System (ADS)

Pestov, Dmitry; Wang, Xi; Ariunbold, Gombojav; Murawski, Robert; Sautenkov, Vladimir; Sokolov, Alexei; Scully, Marlan

2007-10-01

Recent advances in coherent anti-Stokes Raman scattering (CARS) spectroscopy hold exciting promise to make the most out of now readily available ultrafast laser sources. Techniques have been devised to mitigate the nonresonant four-wave-mixing in favor of informative Raman-resonant signal. In particular, a hybrid technique for CARS (see Science 316, 265 (2007)) brings together the advantages of coherent broadband pump-Stokes excitation of molecular vibrations and their time-delayed but frequency-resolved probing via a spectrally narrowed and shaped laser pulse. We apply this technique to the problem of real-time detection of warfare bioagents and report single-shot acquisition of a distinct CARS spectrum from a small volume of B. subtilis endospores (˜10^4 spores), a harmless surrogate for B. anthracis. We study the dependence of the CARS signal on the energy of the ultrashort preparation pulses and find the limit on the pulse energy fluence (˜0.2 J/cm^2), imposed by the laser-induced damage of the spores.

Femtosecond dynamics and laser control of charge transport in trans-polyacetylene.

PubMed

Franco, Ignacio; Shapiro, Moshe; Brumer, Paul

2008-06-28

The induction of dc electronic transport in rigid and flexible trans-polyacetylene oligomers according to the omega versus 2omega coherent control scenario is investigated using a quantum-classical mean field approximation. The approach involves running a large ensemble of mixed quantum-classical trajectories under the influence of omega+2omega laser fields and choosing the initial conditions by sampling the ground-state Wigner distribution function for the nuclei. The vibronic couplings are shown to change the mean single-particle spectrum, introduce ultrafast decoherence, and enhance intramolecular vibrational and electronic relaxation. Nevertheless, even in the presence of significant couplings, limited coherent control of the electronic dynamics is still viable, the most promising route involving the use of femtosecond pulses with a duration that is comparable to the electronic dephasing time. The simulations offer a realistic description of the behavior of a simple coherent control scenario in a complex system and provide a detailed account of the femtosecond photoinduced vibronic dynamics of a conjugated polymer.

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

Relativistic frequency upshift to the extreme ultraviolet regime using self-induced oscillatory flying mirrors

PubMed Central

Kim, I Jong; Pae, Ki Hong; Kim, Chul Min; Kim, Hyung Taek; Yun, Hyeok; Yun, Sang Jae; Sung, Jae Hee; Lee, Seong Ku; Yoon, Jin Woo; Yu, Tae Jun; Jeong, Tae Moon; Nam, Chang Hee; Lee, Jongmin

2012-01-01

Coherent short-wavelength radiation from laser–plasma interactions is of increasing interest in disciplines including ultrafast biomolecular imaging and attosecond physics. Using solid targets instead of atomic gases could enable the generation of coherent extreme ultraviolet radiation with higher energy and more energetic photons. Here we present the generation of extreme ultraviolet radiation through coherent high-harmonic generation from self-induced oscillatory flying mirrors—a new-generation mechanism established in a long underdense plasma on a solid target. Using a 30-fs, 100-TW Ti:sapphire laser, we obtain wavelengths as short as 4.9 nm for an optimized level of amplified spontaneous emission. Particle-in-cell simulations show that oscillatory flying electron nanosheets form in a long underdense plasma, and suggest that the high-harmonic generation is caused by reflection of the laser pulse from electron nanosheets. We expect this extreme ultraviolet radiation to be valuable in realizing a compact X-ray instrument for research in biomolecular imaging and attosecond physics. PMID:23187631

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

NASA Astrophysics Data System (ADS)

Seiler, Hélène; Palato, Samuel; Kambhampati, Patanjali

2017-09-01

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

A final report to the Laboratory Directed Research and Development committee on Project 93-ERP-075: ``X-ray laser propagation and coherence: Diagnosing fast-evolving, high-density laser plasmas using X-ray lasers``

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

Wan, A.S.; Cauble, R.; Da Silva, L.B.

1996-02-01

This report summarizes the major accomplishments of this three-year Laboratory Directed Research and Development (LDRD) Exploratory Research Project (ERP) entitled ``X-ray Laser Propagation and Coherence: Diagnosing Fast-evolving, High-density Laser Plasmas Using X-ray Lasers,`` tracking code 93-ERP-075. The most significant accomplishment of this project is the demonstration of a new laser plasma diagnostic: a soft x-ray Mach-Zehnder interferometer using a neonlike yttrium x-ray laser at 155 {angstrom} as the probe source. Detailed comparisons of absolute two-dimensional electron density profiles obtained from soft x-ray laser interferograms and profiles obtained from radiation hydrodynamics codes, such as LASNEX, will allow us to validate andmore » benchmark complex numerical models used to study the physics of laser-plasma interactions. Thus the development of soft x-ray interferometry technique provides a mechanism to probe the deficiencies of the numerical models and is an important tool for, the high-energy density physics and science-based stockpile stewardship programs. The authors have used the soft x-ray interferometer to study a number of high-density, fast evolving, laser-produced plasmas, such as the dynamics of exploding foils and colliding plasmas. They are pursuing the application of the soft x-ray interferometer to study ICF-relevant plasmas, such as capsules and hohlraums, on the Nova 10-beam facility. They have also studied the development of enhanced-coherence, shorter-pulse-duration, and high-brightness x-ray lasers. The utilization of improved x-ray laser sources can ultimately enable them to obtain three-dimensional holographic images of laser-produced plasmas.« less

Pressure measurements using hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering.

PubMed

Kearney, Sean P; Danehy, Paul M

2015-09-01

We investigate the feasibility of gas-phase pressure measurements using fs/ps rotational CARS. Femtosecond pump and Stokes pulses impulsively prepare a rotational Raman coherence, which is probed by a high-energy 5-ps pulse introduced at a time delay from the Raman preparation. These ultrafast laser pulses are shorter than collisional-dephasing time scales, enabling a new hybrid time- and frequency-domain detection scheme for pressure. Single-laser-shot rotational CARS spectra were recorded from N2 contained in a room-temperature gas cell for pressures from 0.4 to 3 atm and probe delays ranging from 16 to 298 ps. Sensitivity of the accuracy and precision of the pressure data to probe delay was investigated. The technique exhibits superior precision and comparable accuracy to previous laser-diagnostic pressure measurements.

Coupling of a high-energy excitation to superconducting quasiparticles in a cuprate from coherent charge fluctuation spectroscopy

PubMed Central

Mansart, Barbara; Lorenzana, José; Mann, Andreas; Odeh, Ahmad; Scarongella, Mariateresa; Chergui, Majed; Carbone, Fabrizio

2013-01-01

Dynamical information on spin degrees of freedom of proteins or solids can be obtained by NMR and electron spin resonance. A technique with similar versatility for charge degrees of freedom and their ultrafast correlations could move the understanding of systems like unconventional superconductors forward. By perturbing the superconducting state in a high-Tc cuprate, using a femtosecond laser pulse, we generate coherent oscillations of the Cooper pair condensate that can be described by an NMR/electron spin resonance formalism. The oscillations are detected by transient broad-band reflectivity and are found to resonate at the typical scale of Mott physics (2.6 eV), suggesting the existence of a nonretarded contribution to the pairing interaction, as in unconventional (non-Migdal–Eliashberg) theories.

Observation of coherent optical phonons excited by femtosecond laser radiation in Sb films by ultrafast electron diffraction method

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

Mironov, B. N.; Kompanets, V. O.; Aseev, S. A., E-mail: isanfemto@yandex.ru

2017-03-15

The generation of coherent optical phonons in a polycrystalline antimony film sample has been investigated using femtosecond electron diffraction method. Phonon vibrations have been induced in the Sb sample by the main harmonic of a femtosecond Ti:Sa laser (λ = 800 nm) and probed by a pulsed ultrashort photoelectron beam synchronized with the pump laser. The diffraction patterns recorded at different times relative to the pump laser pulse display oscillations of electron diffraction intensity corresponding to the frequencies of vibrations of optical phonons: totally symmetric (A{sub 1g}) and twofold degenerate (E{sub g}) phonon modes. The frequencies that correspond to combinationsmore » of these phonon modes in the Sb sample have also been experimentally observed.« 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.

Ultrafast band-gap oscillations in iron pyrite

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

Kolb, B; Kolpak, AM

2013-12-20

With its combination of favorable band gap, high absorption coefficient, material abundance, and low cost, iron pyrite, FeS2, has received a great deal of attention over the past decades as a promising material for photovoltaic applications such as solar cells and photoelectrochemical cells. Devices made from pyrite, however, exhibit open circuit voltages significantly lower than predicted, and despite a recent resurgence of interest in the material, there currently exists no widely accepted explanation for this disappointing behavior. In this paper, we show that phonons, which have been largely overlooked in previous efforts, may play a significant role. Using fully self-consistentmore » GW calculations, we demonstrate that a phonon mode related to the oscillation of the sulfur-sulfur bond distance in the pyrite structure is strongly coupled to the energy of the conduction-band minimum, leading to an ultrafast (approximate to 100 fs) oscillation in the band gap. Depending on the coherency of the phonons, we predict that this effect can cause changes of up to +/- 0.3 eV relative to the accepted FeS2 band gap at room temperature. Harnessing this effect via temperature or irradiation with infrared light could open up numerous possibilities for novel devices such as ultrafast switches and adaptive solar absorbers.« less

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

DOE PAGES

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

2017-01-09

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

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

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

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

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

Defect-mediated phonon dynamics in TaS2 and WSe2

PubMed Central

Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J.

2017-01-01

We report correlative crystallographic and morphological studies of defect-dependent phonon dynamics in single flakes of 1T-TaS2 and 2H-WSe2 using selected-area diffraction and bright-field imaging in an ultrafast electron microscope. In both materials, we observe in-plane speed-of-sound acoustic-phonon wave trains, the dynamics of which (i.e., emergence, propagation, and interference) are strongly dependent upon discrete interfacial features (e.g., vacuum/crystal and crystal/crystal interfaces). In TaS2, we observe cross-propagating in-plane acoustic-phonon wave trains of differing frequencies that undergo coherent interference approximately 200 ps after initial emergence from distinct interfacial regions. With ultrafast bright-field imaging, the properties of the interfering wave trains are observed to correspond to the beat frequency of the individual oscillations, while intensity oscillations of Bragg spots generated from selected areas within the region of interest match well with the real-space dynamics. In WSe2, distinct acoustic-phonon dynamics are observed emanating and propagating away from structurally dissimilar morphological discontinuities (vacuum/crystal interface and crystal terrace), and results of ultrafast selected-area diffraction reveal thickness-dependent phonon frequencies. The overall observed dynamics are well-described using finite element analysis and time-dependent linear-elastic continuum mechanics. PMID:28503630

Diffraction contrast as a sensitive indicator of femtosecond sub-nanoscale motion in ultrafast transmission electron microscopy

NASA Astrophysics Data System (ADS)

Cremons, Daniel R.; Schliep, Karl B.; Flannigan, David J.

2013-09-01

With ultrafast transmission electron microscopy (UTEM), access can be gained to the spatiotemporal scales required to directly visualize rapid, non-equilibrium structural dynamics of materials. This is achieved by operating a transmission electron microscope (TEM) in a stroboscopic pump-probe fashion by photoelectrically generating coherent, well-timed electron packets in the gun region of the TEM. These probe photoelectrons are accelerated down the TEM column where they travel through the specimen before reaching a standard, commercially-available CCD detector. A second laser pulse is used to excite (pump) the specimen in situ. Structural changes are visualized by varying the arrival time of the pump laser pulse relative to the probe electron packet at the specimen. Here, we discuss how ultrafast nanoscale motions of crystalline materials can be visualized and precisely quantified using diffraction contrast in UTEM. Because diffraction contrast sensitively depends upon both crystal lattice orientation as well as incoming electron wavevector, minor spatial/directional variations in either will produce dynamic and often complex patterns in real-space images. This is because sections of the crystalline material that satisfy the Laue conditions may be heterogeneously distributed such that electron scattering vectors vary over nanoscale regions. Thus, minor changes in either crystal grain orientation, as occurs during specimen tilting, warping, or anisotropic expansion, or in the electron wavevector result in dramatic changes in the observed diffraction contrast. In this way, dynamic contrast patterns observed in UTEM images can be used as sensitive indicators of ultrafast specimen motion. Further, these motions can be spatiotemporally mapped such that direction and amplitude can be determined.

Probing ultra-fast processes with high dynamic range at 4th-generation light sources: Arrival time and intensity binning at unprecedented repetition rates.

PubMed

Kovalev, S; Green, B; Golz, T; Maehrlein, S; Stojanovic, N; Fisher, A S; Kampfrath, T; Gensch, M

2017-03-01

Understanding dynamics on ultrafast timescales enables unique and new insights into important processes in the materials and life sciences. In this respect, the fundamental pump-probe approach based on ultra-short photon pulses aims at the creation of stroboscopic movies. Performing such experiments at one of the many recently established accelerator-based 4th-generation light sources such as free-electron lasers or superradiant THz sources allows an enormous widening of the accessible parameter space for the excitation and/or probing light pulses. Compared to table-top devices, critical issues of this type of experiment are fluctuations of the timing between the accelerator and external laser systems and intensity instabilities of the accelerator-based photon sources. Existing solutions have so far been only demonstrated at low repetition rates and/or achieved a limited dynamic range in comparison to table-top experiments, while the 4th generation of accelerator-based light sources is based on superconducting radio-frequency technology, which enables operation at MHz or even GHz repetition rates. In this article, we present the successful demonstration of ultra-fast accelerator-laser pump-probe experiments performed at an unprecedentedly high repetition rate in the few-hundred-kHz regime and with a currently achievable optimal time resolution of 13 fs (rms). Our scheme, based on the pulse-resolved detection of multiple beam parameters relevant for the experiment, allows us to achieve an excellent sensitivity in real-world ultra-fast experiments, as demonstrated for the example of THz-field-driven coherent spin precession.

Pump-probe study of the formation of rubidium molecules by ultrafast photoassociation of ultracold atoms

NASA Astrophysics Data System (ADS)

McCabe, David J.; England, Duncan G.; Martay, Hugo E. L.; Friedman, Melissa E.; Petrovic, Jovana; Dimova, Emiliya; Chatel, Béatrice; Walmsley, Ian A.

2009-09-01

An experimental pump-probe study of the photoassociative creation of translationally ultracold rubidium molecules is presented together with numerical simulations of the process. The formation of loosely bound excited-state dimers is observed as a first step toward a fully coherent pump-dump approach to the stabilization of Rb2 into its lowest ground vibrational states. The population that contributes to the pump-probe process is characterized and found to be distinct from a background population of preassociated molecules.

Unlocking the Secrets of Brain Signals (4K)

ScienceCinema

None

2018-06-21

Scientists have for the first time determined, at atomic-scale resolution, the 3-D structure of a protein complex that provides the ultrafast trigger for chemicals messages sent between nerve cells in our brains. The discovery, which provides a new understanding of the molecular machinery driving brain function, builds on decades of research at Stanford University, the Stanford School of Medicine and SLAC National Accelerator Laboratory was made possible by SLAC’s Linac Coherent Light Source, an ultrabright X-ray laser.

Unlocking the Secrets of Brain Signals (4K)

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

None

2015-08-17

Scientists have for the first time determined, at atomic-scale resolution, the 3-D structure of a protein complex that provides the ultrafast trigger for chemicals messages sent between nerve cells in our brains. The discovery, which provides a new understanding of the molecular machinery driving brain function, builds on decades of research at Stanford University, the Stanford School of Medicine and SLAC National Accelerator Laboratory was made possible by SLAC’s Linac Coherent Light Source, an ultrabright X-ray laser.

Utility of Modified Ultrafast Papanicolaou Stain in Cytological Diagnosis

PubMed Central

Arakeri, Surekha Ulhas

2017-01-01

Introduction Need for minimal turnaround time for assessing Fine Needle Aspiration Cytology (FNAC) has encouraged innovations in staining techniques that require lesser staining time with unequivocal cell morphology. The standard protocol for conventional Papanicolaou (PAP) stain requires about 40 minutes. To overcome this, Ultrafast Papanicolaou (UFP) stain was introduced which reduces staining time to 90 seconds and also enhances the quality. However, reagents required for this were not easily available hence, Modified Ultrafast Papanicolaou (MUFP) stain was introduced subsequently. Aim To assess the efficacy of MUFP staining by comparing the quality of MUFP stain with conventional PAP stain. Materials and Methods FNAC procedure was performed by using 10 ml disposable syringe and 22-23 G needle. Total 131 FNAC cases were studied which were lymph node (30), thyroid (38), breast (22), skin and soft tissue (24), salivary gland (11) and visceral organs (6). Two smears were prepared and stained by MUFP and conventional PAP stain. Scores were given on four parameters: background of smears, overall staining pattern, cell morphology and nuclear staining. Quality Index (QI) was calculated from ratio of total score achieved to maximum score possible. Statistical analysis using chi square test was applied to each of the four parameters before obtaining the QI in both stains. Students t-test was applied to evaluate the efficacy of MUFP in comparison with conventional PAP stain. Results The QI of MUFP for thyroid, breast, lymph node, skin and soft tissue, salivary gland and visceral organs was 0.89, 0.85, 0.89, 0.83, 0.92, and 0.78 respectively. Compared to conventional PAP stain QI of MUFP smears was better in all except visceral organ cases and was statistically significant. MUFP showed clear red blood cell background, transparent cytoplasm and crisp nuclear features. Conclusion MUFP is fast, reliable and can be done with locally available reagents with unequivocal morphology which is the need of the hour for a cytopathology set-up. PMID:28511391

Utility of Modified Ultrafast Papanicolaou Stain in Cytological Diagnosis.

PubMed

Sinkar, Prachi; Arakeri, Surekha Ulhas

2017-03-01

Need for minimal turnaround time for assessing Fine Needle Aspiration Cytology (FNAC) has encouraged innovations in staining techniques that require lesser staining time with unequivocal cell morphology. The standard protocol for conventional Papanicolaou (PAP) stain requires about 40 minutes. To overcome this, Ultrafast Papanicolaou (UFP) stain was introduced which reduces staining time to 90 seconds and also enhances the quality. However, reagents required for this were not easily available hence, Modified Ultrafast Papanicolaou (MUFP) stain was introduced subsequently. To assess the efficacy of MUFP staining by comparing the quality of MUFP stain with conventional PAP stain. FNAC procedure was performed by using 10 ml disposable syringe and 22-23 G needle. Total 131 FNAC cases were studied which were lymph node (30), thyroid (38), breast (22), skin and soft tissue (24), salivary gland (11) and visceral organs (6). Two smears were prepared and stained by MUFP and conventional PAP stain. Scores were given on four parameters: background of smears, overall staining pattern, cell morphology and nuclear staining. Quality Index (QI) was calculated from ratio of total score achieved to maximum score possible. Statistical analysis using chi square test was applied to each of the four parameters before obtaining the QI in both stains. Students t-test was applied to evaluate the efficacy of MUFP in comparison with conventional PAP stain. The QI of MUFP for thyroid, breast, lymph node, skin and soft tissue, salivary gland and visceral organs was 0.89, 0.85, 0.89, 0.83, 0.92, and 0.78 respectively. Compared to conventional PAP stain QI of MUFP smears was better in all except visceral organ cases and was statistically significant. MUFP showed clear red blood cell background, transparent cytoplasm and crisp nuclear features. MUFP is fast, reliable and can be done with locally available reagents with unequivocal morphology which is the need of the hour for a cytopathology set-up.

Hybrid Hard and Soft Decision Decoding of Reed-Solomon Codes for M-ary Frequency-Shift Keying

DTIC Science & Technology

2010-06-01

Reed-Solomon (RS) coding, Orthogonal signaling, Additive White Gaussian Noise (AWGN), Pulse-Noise Interference (PNI), coherent detection, noncoherent ...Coherent Demodulation of MFSK ....................................................10 2. Noncoherent Demodulation of MFSK...62 V. PERFORMANCE SIMULATION AND ANALYSIS OF MFSK WITH RS ENCODING, HYBRID HD SD DECODING, AND NONCOHERENT DEMODULATION IN AWGN

A first demonstration of audio-frequency optical coherence elastography of tissue

NASA Astrophysics Data System (ADS)

Adie, Steven G.; Alexandrov, Sergey A.; Armstrong, Julian J.; Kennedy, Brendan F.; Sampson, David D.

2008-12-01

Optical elastography is aimed at using the visco-elastic properties of soft tissue as a contrast mechanism, and could be particularly suitable for high-resolution differentiation of tumour from surrounding normal tissue. We present a new approach to measure the effect of an applied stimulus in the kilohertz frequency range that is based on optical coherence tomography. We describe the approach and present the first in vivo optical coherence elastography measurements in human skin at audio excitation frequencies.

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

NASA Astrophysics Data System (ADS)

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

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

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-invasive microscopy in animals and humans using ultrasound. We anticipate that ultrafast ultrasound localization microscopy may become an invaluable tool for the fundamental understanding and diagnostics of various disease processes that modify the microvascular blood flow, such as cancer, stroke and arteriosclerosis.

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-invasive microscopy in animals and humans using ultrasound. We anticipate that ultrafast ultrasound localization microscopy may become an invaluable tool for the fundamental understanding and diagnostics of various disease processes that modify the microvascular blood flow, such as cancer, stroke and arteriosclerosis.

Observation of shock transverse waves in elastic media.

PubMed

Catheline, S; Gennisson, J-L; Tanter, M; Fink, M

2003-10-17

We report the first experimental observation of a shock transverse wave propagating in an elastic medium. This observation was possible because the propagation medium, a soft solid, allows one to reach a very high Mach number. In this extreme configuration, the shock formation is observed over a distance of less than a few wavelengths, thanks to a prototype of an ultrafast scanner (that acquires 5000 frames per second). A comparison of these new experimental data with theoretical predictions, based on a modified Burger's equation, shows good agreement.

Temperature measurements in metalized propellant combustion using hybrid fs/ps coherent anti-Stokes Raman scattering.

PubMed

Kearney, Sean P; Guildenbecher, Daniel R

2016-06-20

We apply ultrafast pure-rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning, aluminized ammonium-perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laser-based diagnostics, with intense background luminosity and scattering from hot metal particles as large as several hundred micrometers in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminum-particle-seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulate-enhanced laser-induced breakdown. Introduction of femtosecond/picosecond (fs/ps) laser pulses improves CARS detection by providing time-gated elimination of strong nonresonant background interference. Single-laser-shot fs/ps CARS spectra were acquired from the burning propellant plume, with picosecond probe-pulse delays of 0 and 16 ps from the femtosecond pump and Stokes pulses. At zero delay, nonresonant background overwhelms the Raman-resonant spectroscopic features. Time-delayed probing results in the acquisition of background-free spectra that were successfully fit for temperature and relative oxygen content. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements with the CARS measurement volume positioned within 3 mm or less of the burning propellant surface. The results show that ultrafast CARS is a potentially enabling technology for probing harsh, particle-laden flame environments.

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.)

Temperature measurements in metalized propellant combustion using hybrid fs/ps coherent anti-Stokes Raman scattering

DOE PAGES

Kearney, Sean P.; Guildenbecher, Daniel R.

2016-06-20

We apply ultrafast pure-rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning, aluminized ammonium-perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laser-based diagnostics, with intense background luminosity and scattering from hot metal particles as large as several hundred micrometers in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminum-particle-seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulate-enhanced laser-induced breakdown. Introduction of femtosecond/picosecond (fs/ps)more » laser pulses improves CARS detection by providing time-gated elimination of strong nonresonant background interference. Single-laser-shot fs/ps CARS spectra were acquired from the burning propellant plume, with picosecond probe-pulse delays of 0 and 16 ps from the femtosecond pump and Stokes pulses. At zero delay, nonresonant background overwhelms the Raman-resonant spectroscopic features. Time-delayed probing results in the acquisition of background-free spectra that were successfully fit for temperature and relative oxygen content. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements with the CARS measurement volume positioned within 3 mm or less of the burning propellant surface. Lastly, the results show that ultrafast CARS is a potentially enabling technology for probing harsh, particle-laden flame environments.« less

Temperature measurements in metalized propellant combustion using hybrid fs/ps coherent anti-Stokes Raman scattering

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

Kearney, Sean P.; Guildenbecher, Daniel R.

We apply ultrafast pure-rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning, aluminized ammonium-perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laser-based diagnostics, with intense background luminosity and scattering from hot metal particles as large as several hundred micrometers in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminum-particle-seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulate-enhanced laser-induced breakdown. Introduction of femtosecond/picosecond (fs/ps)more » laser pulses improves CARS detection by providing time-gated elimination of strong nonresonant background interference. Single-laser-shot fs/ps CARS spectra were acquired from the burning propellant plume, with picosecond probe-pulse delays of 0 and 16 ps from the femtosecond pump and Stokes pulses. At zero delay, nonresonant background overwhelms the Raman-resonant spectroscopic features. Time-delayed probing results in the acquisition of background-free spectra that were successfully fit for temperature and relative oxygen content. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements with the CARS measurement volume positioned within 3 mm or less of the burning propellant surface. Lastly, the results show that ultrafast CARS is a potentially enabling technology for probing harsh, particle-laden flame environments.« less

Ultrafast universal quantum control of a quantum-dot charge qubit using Landau–Zener–Stückelberg interference

PubMed Central

Cao, Gang; Li, Hai-Ou; Tu, Tao; Wang, Li; Zhou, Cheng; Xiao, Ming; Guo, Guang-Can; Jiang, Hong-Wen; Guo, Guo-Ping

2013-01-01

A basic requirement for quantum information processing is the ability to universally control the state of a single qubit on timescales much shorter than the coherence time. Although ultrafast optical control of a single spin has been achieved in quantum dots, scaling up such methods remains a challenge. Here we demonstrate complete control of the quantum-dot charge qubit on the picosecond scale, orders of magnitude faster than the previously measured electrically controlled charge- or spin-based qubits. We observe tunable qubit dynamics in a charge-stability diagram, in a time domain, and in a pulse amplitude space of the driven pulse. The observations are well described by Landau–Zener–Stückelberg interference. These results establish the feasibility of a full set of all-electrical single-qubit operations. Although our experiment is carried out in a solid-state architecture, the technique is independent of the physical encoding of the quantum information and has the potential for wider applications. PMID:23360992

Ultrafast Band Engineering and Transient Spin Currents in Antiferromagnetic Oxides

NASA Astrophysics Data System (ADS)

Gu, Mingqiang; Rondinelli, James M.

2016-04-01

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

Ultrafast Band Engineering and Transient Spin Currents in Antiferromagnetic Oxides.

PubMed

Gu, Mingqiang; Rondinelli, James M

2016-04-29

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

Single-shot measurement of phase and amplitude by using a heterodyne time-lens system and ultrafast digital time-holography

NASA Astrophysics Data System (ADS)

Tikan, Alexey; Bielawski, Serge; Szwaj, Christophe; Randoux, Stéphane; Suret, Pierre

2018-04-01

Temporal imaging systems are outstanding tools for single-shot observation of optical signals that have irregular and ultrafast dynamics. They allow long time windows to be recorded with femtosecond resolution, and do not rely on complex algorithms. However, simultaneous recording of amplitude and phase remains an open challenge for these systems. Here, we present a new heterodyne time-lens arrangement that efficiently records both the amplitude and phase of complex and random signals over large temporal windows (tens of picoseconds). Phase and time are encoded onto the two spatial dimensions of a camera. We implement this phase-sensitive time-lens system in two configurations: a time microscope and a digital temporal-holography device that enables single-shot measurement with a temporal resolution of 80 fs. We demonstrate direct application of our heterodyne time-lens to turbulent-like optical fields and optical rogue waves generated from nonlinear propagation of partially coherent waves inside optical fibres.

Femtosecond X-ray Fourier holography imaging of freeflying nanoparticles

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

Gorkhover, Tais; Ulmer, Anatoli; Ferguson, Ken R.

Ultrafast X-ray imaging on individual fragile specimens such as aerosols1, metastable particles2, superfluid quantum systems3 and live biospecimen4 provides high resolution information, which is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imag- 2 ing, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely-defined4, 5. Here, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers in order to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highestmore » lateral resolution so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond time scale.« less

Wavelength-encoded tomography based on optical temporal Fourier transform

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

Zhang, Chi; Wong, Kenneth K. Y., E-mail: kywong@eee.hku.hk

We propose and demonstrate a technique called wavelength-encoded tomography (WET) for non-invasive optical cross-sectional imaging, particularly beneficial in biological system. The WET utilizes time-lens to perform the optical Fourier transform, and the time-to-wavelength conversion generates a wavelength-encoded image of optical scattering from internal microstructures, analogous to the interferometery-based imaging such as optical coherence tomography. Optical Fourier transform, in principle, comes with twice as good axial resolution over the electrical Fourier transform, and will greatly simplify the digital signal processing after the data acquisition. As a proof-of-principle demonstration, a 150 -μm (ideally 36 μm) resolution is achieved based on a 7.5-nm bandwidth swept-pump,more » using a conventional optical spectrum analyzer. This approach can potentially achieve up to 100-MHz or even higher frame rate with some proven ultrafast spectrum analyzer. We believe that this technique is innovative towards the next-generation ultrafast optical tomographic imaging application.« less

Theory of low-power ultra-broadband terahertz sideband generation in bi-layer graphene.

PubMed

Crosse, J A; Xu, Xiaodong; Sherwin, Mark S; Liu, R B

2014-09-24

In a semiconductor illuminated by a strong terahertz (THz) field, optically excited electron-hole pairs can recombine to emit light in a broad frequency comb evenly spaced by twice the THz frequency. Such high-order THz sideband generation is of interest both as an example of extreme nonlinear optics and also as a method for ultrafast electro-optical modulation. So far, this phenomenon has only been observed with large field strengths (~10 kV cm(-1)), an obstacle for technological applications. Here we predict that bi-layer graphene generates high-order sidebands at much weaker THz fields. We find that a THz field of strength 1 kV cm(-1) can produce a high-sideband spectrum of about 30 THz, 100 times broader than in GaAs. The sidebands are generated despite the absence of classical collisions, with the quantum coherence of the electron-hole pairs enabling recombination. These remarkable features lower the barrier to desktop electro-optical modulation at THz frequencies, facilitating ultrafast optical communications.

Ultrafast band engineering and transient spin currents in antiferromagnetic oxides

DOE PAGES

Gu, Mingqiang; Rondinelli, James M.

2016-04-29

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

Femtosecond electron imaging of defect-modulated phonon dynamics

PubMed Central

Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J.

2016-01-01

Precise manipulation and control of coherent lattice oscillations via nanostructuring and phonon-wave interference has the potential to significantly impact a broad array of technologies and research areas. Resolving the dynamics of individual phonons in defect-laden materials presents an enormous challenge, however, owing to the interdependent nanoscale and ultrafast spatiotemporal scales. Here we report direct, real-space imaging of the emergence and evolution of acoustic phonons at individual defects in crystalline WSe2 and Ge. Via bright-field imaging with an ultrafast electron microscope, we are able to image the sub-picosecond nucleation and the launch of wavefronts at step edges and resolve dispersion behaviours during propagation and scattering. We discover that the appearance of speed-of-sound (for example, 6 nm ps−1) wavefronts are influenced by spatially varying nanoscale strain fields, taking on the appearance of static bend contours during propagation. These observations provide unprecedented insight into the roles played by individual atomic and nanoscale features on acoustic-phonon dynamics. PMID:27079790

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

PubMed Central

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

2017-01-01

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

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

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

Albert, Felicie

2016-10-12

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

Ultrafast Band Engineering and Transient Spin Currents in Antiferromagnetic Oxides

PubMed Central

Gu, Mingqiang; Rondinelli, James M.

2016-01-01

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

Detuning dependence of Rabi oscillations in an InAs self-assembled quantum dot ensemble

NASA Astrophysics Data System (ADS)

Suzuki, Takeshi; Singh, Rohan; Bayer, Manfred; Ludzwig, Arne; Wieck, Andreas D.; Cundiff, Steven T.

2018-04-01

We study the coherent evolution of an InAs self-assembled quantum dot (QD) ensemble in the ultrafast regime. The evolution of the entire frequency distribution is revealed by performing prepulse two-dimensional (2D) coherent spectroscopy. Charged and neutral QDs display distinct nonlinear responses arising from two-level trion and four-level exciton-biexciton systems, respectively, and each signal is clearly separated in 2D spectra. Whereas the signals for charged QDs are symmetric with respect to the detuning, those for neutral QDs are asymmetric due to the asymmetric four-level energy structure. Experimental results for charged and neutral QDs are well reproduced by solving the optical Bloch equations, including detuning and excitation-induced dephasing (EID) effects. The temperature dependence suggests that wetting-layer carriers play an important role in EID.

Resonant soft X-ray scattering for polymer materials

DOE PAGES

Liu, Feng; Brady, Michael A.; Wang, Cheng

2016-04-16

Resonant Soft X-ray Scattering (RSoXS) was developed within the last few years, and the first dedicated resonant soft X-ray scattering beamline for soft materials was constructed at the Advanced Light Source, LBNL. RSoXS combines soft X-ray spectroscopy with X-ray scattering and thus offers statistical information for 3D chemical morphology over a large length scale range from nanometers to micrometers. Using RSoXS to characterize multi-length scale soft materials with heterogeneous chemical structures, we have demonstrated that soft X-ray scattering is a unique complementary technique to conventional hard X-ray and neutron scattering. Its unique chemical sensitivity, large accessible size scale, molecular bondmore » orientation sensitivity with polarized X-rays, and high coherence have shown great potential for chemically specific structural characterization for many classes of materials.« less

Numerical simulation of a soft-x-ray Li laser pumped with synchrotron radiation

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

Rozsnyai, B.; Watanabe, H.; Csonka, P.L.

1985-07-01

Results of a computer simulation are reported for a lithium soft-x-ray laser pumped by synchro- tron radiation. Coherent stimulated emission of the photons of interest occurs in Li II 1s2p..-->..Li II 1s/sup 2/ transitions. Calculated results include the dominant ion and photon densities and the laser gain.

A study of coherence of soft gluons in hadron jets

NASA Astrophysics Data System (ADS)

Akrawy, M. Z.; Alexander, G.; Allison, J.; Allport, P. P.; Anderson, K. J.; Armitage, J. C.; Arnison, G. T. J.; Ashton, P.; Azuelos, G.; Baines, J. T. M.; Ball, A. H.; Banks, J.; Barker, G. J.; Barlow, R. J.; Batley, J. R.; Becker, J.; Behnke, T.; Bell, K. W.; Bella, G.; Bethke, S.; Biebel, O.; Binder, U.; Bloodworth, I. J.; Bock, P.; Breuker, H.; Brown, R. M.; Brun, R.; Buijs, A.; Burckhart, H. J.; Capiluppi, P.; Carnegie, R. K.; Carter, A. A.; Carter, J. R.; Chang, C. Y.; Charlton, D. G.; Chrin, J. T. M.; Clarke, P. E. L.; Cohen, I.; Collins, W. J.; Conboy, J. E.; Couch, M.; Coupland, M.; Cuffiani, M.; Dado, S.; Dallavalle, G. M.; Debu, P.; Deninno, M. M.; Dieckmann, A.; Dittmar, M.; Dixit, M. S.; Duchovni, E.; Duerdoth, I. P.; Dumas, D. J. P.; El Mamouni, H.; Elcombe, P. A.; Estabrooks, P. G.; Etzion, E.; Fabbri, F.; Farthouat, P.; Fischer, H. M.; Fong, D. G.; French, M. T.; Fukunaga, C.; Gaidot, A.; Ganel, O.; Gary, J. W.; Gascon, J.; Geddes, N. I.; Gee, C. N. P.; Geich-Gimbel, C.; Gensler, S. W.; Gentit, F. X.; Giacomelli, G.; Gibson, V.; Gibson, W. R.; Gillies, J. D.; Goldberg, J.; Goodrick, M. J.; Gorn, W.; Granite, D.; Gross, E.; Grunhaus, J.; Hagedorn, H.; Hagemann, J.; Hansroul, M.; Hargrove, C. K.; Harrus, I.; Hart, J.; Hattersley, P. M.; Hauschild, M.; Hawkes, C. M.; Heflin, E.; Hemingway, R. J.; Heuer, R. D.; Hill, J. C.; Hillier, S. J.; Ho, C.; Hobbs, J. D.; Hobson, P. R.; Hochman, D.; Holl, B.; Homer, R. J.; Hou, S. R.; Howarth, C. P.; Hughes-Jones, R. E.; Humbert, R.; Igo-Kemenes, P.; Ihssen, H.; Imrie, D. C.; Jawahery, A.; Jeffreys, P. W.; Jeremie, H.; Jimack, M.; Jobes, M.; Jones, R. W. L.; Jovanovic, P.; Karlen, D.; Kawagoe, K.; Kawamoto, T.; Kellogg, R. G.; Kennedy, B. W.; Kleinwort, C.; Klem, D. E.; Knop, G.; Kobayashi, T.; Kokott, T. P.; Köpke, L.; Kowalewski, R.; Kreutzmann, H.; Kroll, J.; Kuwano, M.; Kyberd, P.; Lafferty, G. D.; Lamarche, F.; Larson, W. J.; Layter, J. G.; Le Du, P.; Leblanc, P.; Lee, A. M.; Lehto, M. H.; Lellouch, D.; Lennert, P.; Lessard, L.; Levinson, L.; Lloyd, S. L.; Loebinger, F. K.; Lorah, J. M.; Lorazo, B.; Losty, M. J.; Ludwig, J.; Ma, J.; Macbeth, A. A.; Mannelli, M.; Marcellini, S.; Maringer, G.; Martin, A. J.; Martin, J. P.; Mashimo, T.; Mättig, P.; Maur, U.; McMahon, T. J.; McNutt, J. R.; McPherson, A. C.; Meijers, F.; Menszner, D.; Merritt, F. S.; Mes, H.; Michelini, A.; Middleton, R. P.; Mikenberg, G.; Miller, D. J.; Milstene, C.; Minowa, M.; Mohr, W.; Montanari, A.; Mori, T.; Moss, M. W.; Murphy, P. G.; Murray, W. J.; Nellen, B.; Nguyen, H. H.; Nozaki, M.; O'Dowd, A. J. P.; O'Neale, S. W.; O'Neill, B. P.; Oakham, F. G.; Odorici, F.; Ogg, M.; Oh, H.; Oreglia, M. J.; Orito, S.; Pansart, J. P.; Patrick, G. N.; Pawley, S. J.; Pfister, P.; Pilcher, J. E.; Pinfold, J. L.; Plane, D. E.; Poli, B.; Pouladdej, A.; Pritchard, T. W.; Quast, G.; Raab, J.; Redmond, M. W.; Rees, D. L.; Regimbald, M.; Riles, K.; Roach, C. M.; Robins, S. A.; Rollnik, A.; Roney, J. M.; Rossberg, S.; Rossi, A. M.; Routenburg, P.; Runge, K.; Runolfsson, O.; Sanghera, S.; Sansum, R. A.; Sasaki, M.; Saunders, B. J.; Schaile, A. D.; Schaile, O.; Schappert, W.; Scharff-Hansen, P.; Schreiber, S.; Schwarz, J.; Shapira, A.; Shen, B. C.; Sherwood, P.; Simon, A.; Singh, P.; Siroli, G. P.; Skuia, A.; Smith, A. M.; Smith, T. J.; Snow, G. A.; Springer, R. W.; Sproston, M.; Stephens, K.; Stier, H. E.; Ströhmer, R.; Strom, D.; Takeda, H.; Takeshita, T.; Tsukamoto, T.; Turner, M. F.; Tysarczyk-Niemeyer, G.; Van den plas, D.; VanDalen, G. J.; Vasseur, G.; Virtue, C. J.; von der Schmitt, H.; von Krogh, J.; Wagner, A.; Wahl, C.; Ward, C. P.; Ward, D. R.; Waterhouse, J.; Watkins, P. M.; Watson, A. T.; Watson, N. K.; Weber, M.; Weisz, S.; Wells, P. S.; Wermes, N.; Weymann, M.; Wilson, G. W.; Wilson, J. A.; Wingerter, I.; Winterer, V.-H.; Wood, N. C.; Wotton, S.; Wuensch, B.; Wyatt, T. R.; Yaari, R.; Yang, Y.; Yekutieli, G.; Yoshida, T.; Zeuner, W.; Zorn, G. T.; OPAL Collaboration

1990-09-01

We study the inclusive momentum distribution of charged particles in multihadronic events produced in e +e - annihilations at ECM∼ M(Z 0). We find agreement with the analytical formulae for gluon production that include the phenomena of soft gluon interference. Using data from CM energies between 14 and 91 GeV, we study the dependence of the inclusive momentum distribution on the centre of momentum energy. We find that the analytical formulae describe the data over the entire energy range. Both the momentum distribution at a fixed energy and the change with energy are described by QCD shower Monte Carlo's which include either coherent gluon branchings or string fragmentation. Simple incoherent models with independent fragmentation fail to reproduce the energy dependence and momentum spectra.

Multiobjective optimization design of an rf gun based electron diffraction beam line

NASA Astrophysics Data System (ADS)

Gulliford, Colwyn; Bartnik, Adam; Bazarov, Ivan; Maxson, Jared

2017-03-01

Multiobjective genetic algorithm optimizations of a single-shot ultrafast electron diffraction beam line comprised of a 100 MV /m 1.6-cell normal conducting rf (NCRF) gun, as well as a nine-cell 2 π /3 bunching cavity placed between two solenoids, have been performed. These include optimization of the normalized transverse emittance as a function of bunch charge, as well as optimization of the transverse coherence length as a function of the rms bunch length of the beam at the sample location for a fixed charge of 1 06 electrons. Analysis of the resulting solutions is discussed in terms of the relevant scaling laws, and a detailed description of one of the resulting solutions from the coherence length optimizations is given. For a charge of 1 06 electrons and final beam sizes of σx≥25 μ m and σt≈5 fs , we found a relative coherence length of Lc ,x/σx≈0.07 using direct optimization of the coherence length. Additionally, based on optimizations of the emittance as a function of final bunch length, we estimate the relative coherence length for bunch lengths of 30 and 100 fs to be roughly 0.1 and 0.2 nm /μ m , respectively. Finally, using the scaling of the optimal emittance with bunch charge, for a charge of 1 05 electrons, we estimate relative coherence lengths of 0.3, 0.5, and 0.92 nm /μ m for final bunch lengths of 5, 30 and 100 fs, respectively.

Ultrafast dynamics during the photoinduced phase transition in VO2

NASA Astrophysics Data System (ADS)

Wegkamp, Daniel; Stähler, Julia

2015-12-01

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

Probing ultra-fast processes with high dynamic range at 4th-generation light sources: Arrival time and intensity binning at unprecedented repetition rates

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

Kovalev, S.; Green, B.; Golz, T.

Here, understanding dynamics on ultrafast timescales enables unique and new insights into important processes in the materials and life sciences. In this respect, the fundamental pump-probe approach based on ultra-short photon pulses aims at the creation of stroboscopic movies. Performing such experiments at one of the many recently established accelerator-based 4th-generation light sources such as free-electron lasers or superradiant THz sources allows an enormous widening of the accessible parameter space for the excitation and/or probing light pulses. Compared to table-top devices, critical issues of this type of experiment are fluctuations of the timing between the accelerator and external laser systemsmore » and intensity instabilities of the accelerator-based photon sources. Existing solutions have so far been only demonstrated at low repetition rates and/or achieved a limited dynamic range in comparison to table-top experiments, while the 4th generation of accelerator-based light sources is based on superconducting radio-frequency technology, which enables operation at MHz or even GHz repetition rates. In this article, we present the successful demonstration of ultra-fast accelerator-laser pump-probe experiments performed at an unprecedentedly high repetition rate in the few-hundred-kHz regime and with a currently achievable optimal time resolution of 13 fs (rms). Our scheme, based on the pulse-resolved detection of multiple beam parameters relevant for the experiment, allows us to achieve an excellent sensitivity in real-world ultra-fast experiments, as demonstrated for the example of THz-field-driven coherent spin precession.« less

Probing ultra-fast processes with high dynamic range at 4th-generation light sources: Arrival time and intensity binning at unprecedented repetition rates

DOE PAGES

Kovalev, S.; Green, B.; Golz, T.; ...

2017-03-06

Here, understanding dynamics on ultrafast timescales enables unique and new insights into important processes in the materials and life sciences. In this respect, the fundamental pump-probe approach based on ultra-short photon pulses aims at the creation of stroboscopic movies. Performing such experiments at one of the many recently established accelerator-based 4th-generation light sources such as free-electron lasers or superradiant THz sources allows an enormous widening of the accessible parameter space for the excitation and/or probing light pulses. Compared to table-top devices, critical issues of this type of experiment are fluctuations of the timing between the accelerator and external laser systemsmore » and intensity instabilities of the accelerator-based photon sources. Existing solutions have so far been only demonstrated at low repetition rates and/or achieved a limited dynamic range in comparison to table-top experiments, while the 4th generation of accelerator-based light sources is based on superconducting radio-frequency technology, which enables operation at MHz or even GHz repetition rates. In this article, we present the successful demonstration of ultra-fast accelerator-laser pump-probe experiments performed at an unprecedentedly high repetition rate in the few-hundred-kHz regime and with a currently achievable optimal time resolution of 13 fs (rms). Our scheme, based on the pulse-resolved detection of multiple beam parameters relevant for the experiment, allows us to achieve an excellent sensitivity in real-world ultra-fast experiments, as demonstrated for the example of THz-field-driven coherent spin precession.« less

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

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

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

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.

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

DOE PAGES

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung; ...

2017-05-24

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

Temperature-dependence of hypersound dynamics in SrTiO3/SrRuO3 heterostructures studied by ultrafast spectroscopy

NASA Astrophysics Data System (ADS)

Yang, Chi-Yuan; Yadav, Ajay K.; Ramesh, Ramamoorthy; Wen, Yu-Chieh; Hsu, Chia-Hao; Wu, Maw-Kuen; Chia, Chih-Ta; Lin, Kung-Hsuan

Strontium titanate (SrTiO3, STO) and strontium ruthenate (SrRuO3, SRO) are complex oxide with perovskite structure. Their property, such as thermoelectricity and superconductivity, has been widely investigated for scientific and industrial purposes. Recently, complex oxide heterostructures can be grown by pulsed laser deposition. It opens many possibilities f or new properties of materials. With ultrafast pump-probe spectroscopy, we demonstrated that metal-like SRO thin film can be served as a phonon transducer to generate hypersound with frequency of several tens to several hundreads of GHz. This technique can be utilized to study not only the elastic properties of perovskite thin films but also the interfaces. In this study, we used this technique to study the temperature dependence of structural phases in STO. During the crossing over the soft-mode transition in STO around 110 K, the shortening of phonon lifetime were also observed.

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

NASA Astrophysics Data System (ADS)

Tisdale, William A., III

Finding a viable supply of clean, renewable energy is one of the most daunting challenges facing the world today. Solar cells have had limited impact in meeting this challenge because of their high cost and low power conversion efficiencies. Semiconductor nanocrystals, or quantum dots, are promising materials for use in novel solar cells because they can be processed with potentially inexpensive solution-based techniques and because they are predicted to have novel optoelectronic properties that could enable the realization of ultra-efficient solar power converters. However, there is a lack of fundamental understanding regarding the behavior of highly-excited, or "hot," charge carriers near quantum-dot and semiconductor interfaces, which is of paramount importance to the rational design of high-efficiency devices. The elucidation of these ultrafast hot electron dynamics is the central aim of this Dissertation. I present a theoretical framework for treating the electronic interactions between quantum dots and bulk semiconductor surfaces and propose a novel experimental technique, time-resolved surface second harmonic generation (TR-SHG), for probing these interactions. I then describe a series of experimental investigations into hot electron dynamics in specific quantum-dot/semiconductor systems. A two-photon photoelectron spectroscopy (2PPE) study of the technologically-relevant ZnO(1010) surface reveals ultrafast (sub-30fs) cooling of hot electrons in the bulk conduction band, which is due to strong electron-phonon coupling in this highly polar material. The presence of a continuum of defect states near the conduction band edge results in Fermi-level pinning and upward (n-type) band-bending at the (1010) surface and provides an alternate route for electronic relaxation. In monolayer films of colloidal PbSe quantum dots, chemical treatment with either hydrazine or 1,2-ethanedithiol results in strong and tunable electronic coupling between neighboring quantum dots. 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.

Coherent quantum dynamics launched by incoherent relaxation in a quantum circuit simulator of a light-harvesting complex

NASA Astrophysics Data System (ADS)

Chin, A. W.; Mangaud, E.; Atabek, O.; Desouter-Lecomte, M.

2018-06-01

Engineering and harnessing coherent excitonic transport in organic nanostructures has recently been suggested as a promising way towards improving manmade light-harvesting materials. However, realizing and testing the dissipative system-environment models underlying these proposals is presently very challenging in supramolecular materials. A promising alternative is to use simpler and highly tunable "quantum simulators" built from programmable qubits, as recently achieved in a superconducting circuit by Potočnik et al. [A. Potočnik et al., Nat. Commun. 9, 904 (2018), 10.1038/s41467-018-03312-x]. We simulate the real-time dynamics of an exciton coupled to a quantum bath as it moves through a network based on the quantum circuit of Potočnik et al. Using the numerically exact hierarchical equations of motion to capture the open quantum system dynamics, we find that an ultrafast but completely incoherent relaxation from a high-lying "bright" exciton into a doublet of closely spaced "dark" excitons can spontaneously generate electronic coherences and oscillatory real-space motion across the network (quantum beats). Importantly, we show that this behavior also survives when the environmental noise is classically stochastic (effectively high temperature), as in present experiments. These predictions highlight the possibilities of designing matched electronic and spectral noise structures for robust coherence generation that do not require coherent excitation or cold environments.

Infrared laser damage thresholds in corneal tissue phantoms using femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Boretsky, Adam R.; Clary, Joseph E.; Noojin, Gary D.; Rockwell, Benjamin A.

2018-02-01

Ultrafast lasers have become a fixture in many biomedical, industrial, telecommunications, and defense applications in recent years. These sources are capable of generating extremely high peak power that can cause laser-induced tissue breakdown through the formation of a plasma upon exposure. Despite the increasing prevalence of such lasers, current safety standards (ANSI Z136.1-2014) do not include maximum permissible exposure (MPE) values for the cornea with pulse durations less than one nanosecond. This study was designed to measure damage thresholds in corneal tissue phantoms in the near-infrared and mid-infrared to identify the wavelength dependence of laser damage thresholds from 1200-2500 nm. A high-energy regenerative amplifier and optical parametric amplifier outputting 100 femtosecond pulses with pulse energies up to 2 mJ were used to perform exposures and determine damage thresholds in transparent collagen gel tissue phantoms. Three-dimensional imaging, primarily optical coherence tomography, was used to evaluate tissue phantoms following exposure to determine ablation characteristics at the surface and within the bulk material. The determination of laser damage thresholds in the near-IR and mid-IR for ultrafast lasers will help to guide safety standards and establish the appropriate MPE levels for exposure sensitive ocular tissue such as the cornea. These data will help promote the safe use of ultrafast lasers for a wide range of applications.

Strong-Field Control of Laser Filamentation Mechanisms

NASA Astrophysics Data System (ADS)

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

2008-05-01

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

Ultrafast 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.

Terahertz emission from ultrafast ionizing air in symmetry-broken laser fields

NASA Astrophysics Data System (ADS)

Kim, Ki-Yong; Glownia, James H.; Taylor, Antoinette J.; Rodriguez, George

2007-04-01

A transient photocurrent model is developed to explain coherent terahertz emission from air irradiated by a symmetry-broken laser field composed of the fundamental and its second harmonic laser pulses. When the total laser field is asymmetric across individual optical cycles, a nonvanishing electron current surge can arise during optical field ionization of air, emitting a terahertz electromagnetic pulse. Terahertz power scalability is also investigated, and with optical pump energy of tens of millijoules per pulse, peak terahertz field strengths in excess of 150 kV/cm are routinely produced.

Terahertz emission from ultrafast ionizing air in symmetry-broken laser fields.

PubMed

Kim, Ki-Yong; Glownia, James H; Taylor, Antoinette J; Rodriguez, George

2007-04-16

A transient photocurrent model is developed to explain coherent terahertz emission from air irradiated by a symmetry-broken laser field composed of the fundamental and its second harmonic laser pulses. When the total laser field is asymmetric across individual optical cycles, a nonvanishing electron current surge can arise during optical field ionization of air, emitting a terahertz electromagnetic pulse. Terahertz power scalability is also investigated, and with optical pump energy of tens of millijoules per pulse, peak terahertz field strengths in excess of 150 kV/cm are routinely produced.

The X-ray Pump–Probe instrument at the Linac Coherent Light Source

DOE PAGES

Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco; ...

2015-04-21

The X-ray Pump–Probe instrument achieves femtosecond time-resolution with hard X-ray methods using a free-electron laser source. It covers a photon energy range of 4–24 keV. A femtosecond optical laser system is available across a broad spectrum of wavelengths for generating transient states of matter. The instrument is designed to emphasize versatility and the scientific goals encompass ultrafast physical, chemical and biological processes involved in the transformation of matter and transfer of energy at the atomic scale.

Influence of Processing Additives on Charge-Transfer Time Scales and Sound Velocity in Organic Bulk Heterojunction Films.

PubMed

Kaake, Loren G; Welch, Gregory C; Moses, Daniel; Bazan, Guillermo C; Heeger, Alan J

2012-05-17

The role of processing additives in organic bulk heterojunction thin films was investigated by means of transient absorption spectroscopy. The rate of ultrafast charge transfer was found to increase when a small amount of diiodooctane was used during film formation. In addition, coherent acoustic phonons were observed, and their velocity was determined. A strong correlation between the sound velocity and the charge-transfer time scale was observed, both of which could be explained by a subtle increase in thin film density.

Strong-field two-photon transition by phase shaping

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

Lee, Sangkyung; Lim, Jongseok; Ahn, Jaewook

2010-08-15

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

The X-ray Pump-Probe instrument at the Linac Coherent Light Source.

PubMed

Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco; Damiani, Daniel; Defever, Jim; Delor, James T; Feng, Yiping; Glownia, James M; Langton, J Brian; Nelson, Silke; Ramsey, Kelley; Robert, Aymeric; Sikorski, Marcin; Song, Sanghoon; Stefanescu, Daniel; Srinivasan, Venkat; Zhu, Diling; Lemke, Henrik T; Fritz, David M

2015-05-01

The X-ray Pump-Probe instrument achieves femtosecond time-resolution with hard X-ray methods using a free-electron laser source. It covers a photon energy range of 4-24 keV. A femtosecond optical laser system is available across a broad spectrum of wavelengths for generating transient states of matter. The instrument is designed to emphasize versatility and the scientific goals encompass ultrafast physical, chemical and biological processes involved in the transformation of matter and transfer of energy at the atomic scale.

Hyperspectral microscopic imaging by multiplex coherent anti-Stokes Raman scattering (CARS)

NASA Astrophysics Data System (ADS)

Khmaladze, Alexander; Jasensky, Joshua; Zhang, Chi; Han, Xiaofeng; Ding, Jun; Seeley, Emily; Liu, Xinran; Smith, Gary D.; Chen, Zhan

2011-10-01

Coherent anti-Stokes Raman scattering (CARS) microscopy is a powerful technique to image the chemical composition of complex samples in biophysics, biology and materials science. CARS is a four-wave mixing process. The application of a spectrally narrow pump beam and a spectrally wide Stokes beam excites multiple Raman transitions, which are probed by a probe beam. This generates a coherent directional CARS signal with several orders of magnitude higher intensity relative to spontaneous Raman scattering. Recent advances in the development of ultrafast lasers, as well as photonic crystal fibers (PCF), enable multiplex CARS. In this study, we employed two scanning imaging methods. In one, the detection is performed by a photo-multiplier tube (PMT) attached to the spectrometer. The acquisition of a series of images, while tuning the wavelengths between images, allows for subsequent reconstruction of spectra at each image point. The second method detects CARS spectrum in each point by a cooled coupled charged detector (CCD) camera. Coupled with point-by-point scanning, it allows for a hyperspectral microscopic imaging. We applied this CARS imaging system to study biological samples such as oocytes.

Near- and Extended-Edge X-Ray-Absorption Fine-Structure Spectroscopy Using Ultrafast Coherent High-Order Harmonic Supercontinua

NASA Astrophysics Data System (ADS)

Popmintchev, Dimitar; Galloway, Benjamin R.; Chen, Ming-Chang; Dollar, Franklin; Mancuso, Christopher A.; Hankla, Amelia; Miaja-Avila, Luis; O'Neil, Galen; Shaw, Justin M.; Fan, Guangyu; Ališauskas, Skirmantas; Andriukaitis, Giedrius; Balčiunas, Tadas; Mücke, Oliver D.; Pugzlys, Audrius; Baltuška, Andrius; Kapteyn, Henry C.; Popmintchev, Tenio; Murnane, Margaret M.

2018-03-01

Recent advances in high-order harmonic generation have made it possible to use a tabletop-scale setup to produce spatially and temporally coherent beams of light with bandwidth spanning 12 octaves, from the ultraviolet up to x-ray photon energies >1.6 keV . Here we demonstrate the use of this light for x-ray-absorption spectroscopy at the K - and L -absorption edges of solids at photon energies near 1 keV. We also report x-ray-absorption spectroscopy in the water window spectral region (284-543 eV) using a high flux high-order harmonic generation x-ray supercontinuum with 109 photons/s in 1% bandwidth, 3 orders of magnitude larger than has previously been possible using tabletop sources. Since this x-ray radiation emerges as a single attosecond-to-femtosecond pulse with peak brightness exceeding 1026 photons/s /mrad2/mm2/1 % bandwidth, these novel coherent x-ray sources are ideal for probing the fastest molecular and materials processes on femtosecond-to-attosecond time scales and picometer length scales.

Attosecond Light and Science at the Time-scale of the Electron - Coherent X-Rays from Tabletop Ultrafast Lasers

ScienceCinema

Margaret, Murnane [University of Colorado, Boulder and NIST

2017-12-09

Ever since the invention of the laser 50 years ago and its application in nonlinear optics, scientists have been striving to extend coherent laser beams into the x-ray region of the spectrum. Very recently however, the prospects for tabletop coherent sources at very short wavelengths, even in the hard x-ray region of the spectrum at wavelengths < 1nm, have brightened considerably. This advance is possible by taking nonlinear optics techniques to an extreme - physics that is the direct result of a new ability to manipulate electrons on the fastest, attosecond, time-scales of our natural world. Several applications have already been demonstrated, including making a movie of how electrons rearrange in a chemical bond changes shape as a molecule breaks apart, following how fast a magnetic material can flip orientation, understanding how fast heat flows in a nanocircuit, or building a microscope without lenses. Nature 460, 1088 (2009); Science 317, 775 (2007); Physical Review Letters 103, 257402 (2009); Nature Materials 9, 26 (2010); Nature 463, 214 (2010); Science 322, 1207 (2008).

Coherent diffractive imaging of single helium nanodroplets with a high harmonic generation source.

PubMed

Rupp, Daniela; Monserud, Nils; Langbehn, Bruno; Sauppe, Mario; Zimmermann, Julian; Ovcharenko, Yevheniy; Möller, Thomas; Frassetto, Fabio; Poletto, Luca; Trabattoni, Andrea; Calegari, Francesca; Nisoli, Mauro; Sander, Katharina; Peltz, Christian; J Vrakking, Marc; Fennel, Thomas; Rouzée, Arnaud

2017-09-08

Coherent diffractive imaging of individual free nanoparticles has opened routes for the in situ analysis of their transient structural, optical, and electronic properties. So far, single-shot single-particle diffraction was assumed to be feasible only at extreme ultraviolet and X-ray free-electron lasers, restricting this research field to large-scale facilities. Here we demonstrate single-shot imaging of isolated helium nanodroplets using extreme ultraviolet pulses from a femtosecond-laser-driven high harmonic source. We obtain bright wide-angle scattering patterns, that allow us to uniquely identify hitherto unresolved prolate shapes of superfluid helium droplets. Our results mark the advent of single-shot gas-phase nanoscopy with lab-based short-wavelength pulses and pave the way to ultrafast coherent diffractive imaging with phase-controlled multicolor fields and attosecond pulses.Diffraction imaging studies of free individual nanoparticles have so far been restricted to XUV and X-ray free - electron laser facilities. Here the authors demonstrate the possibility of using table-top XUV laser sources to image prolate shapes of superfluid helium droplets.

Experimental demonstration of a soft x-ray self-seeded free-electron laser

DOE PAGES

Ratner, D.; Abela, R.; Amann, J.; ...

2015-02-06

The Linac Coherent Light Source has added self-seeding capability to the soft x-ray range using a grating monochromator system. We report demonstration of soft x-ray self-seeding with a measured resolving power of 2000-5000, wavelength stability of 10 -4, and an increase in peak brightness by a factor of 2-5 across the photon energy range of 500-1000 eV. By avoiding the need for a monochromator at the experimental station, the self-seeded beam can deliver as much as 50 fold higher brightness to users.

Development and calibration of mirrors and gratings for the Soft X-ray materials science beamline at the Linac Coherent Light Source free-electron laser

DOE PAGES

Soufli, Regina; Fernandez-Perea, Monica; Baker, Sherry L.; ...

2012-04-18

This article discusses the development and calibration of the x-ray reflective and diffractive elements for the Soft X-ray Materials Science (SXR) beamline of the Linac Coherent Light Source (LCLS) free-electron laser (FEL), designed for operation in the 500 – 2000 eV region. The surface topography of three Si mirror substrates and two Si diffraction grating substrates was examined by atomic force microscopy (AFM) and optical profilometry. The figure of the mirror substrates was also verified via surface slope measurements with a long trace profiler. A boron carbide (B 4C) coating especially optimized for the LCLS FEL conditions was deposited onmore » all SXR mirrors and gratings. Coating thickness uniformity of 0.14 nm root mean square (rms) across clear apertures extending to 205 mm length was demonstrated for all elements, as required to preserve the coherent wavefront of the LCLS source. The reflective performance of the mirrors and the diffraction efficiency of the gratings were calibrated at beamline 6.3.2 at the Advanced Light Source synchrotron. To verify the integrity of the nanometer-scale grating structure, the grating topography was examined by AFM before and after coating. This is to our knowledge the first time B 4C-coated diffraction gratings are demonstrated for operation in the soft x-ray region.« less

4D electron microscopy: principles and applications.

PubMed

Flannigan, David J; Zewail, Ahmed H

2012-10-16

The transmission electron microscope (TEM) is a powerful tool enabling the visualization of atoms with length scales smaller than the Bohr radius at a factor of only 20 larger than the relativistic electron wavelength of 2.5 pm at 200 keV. The ability to visualize matter at these scales in a TEM is largely due to the efforts made in correcting for the imperfections in the lens systems which introduce aberrations and ultimately limit the achievable spatial resolution. In addition to the progress made in increasing the spatial resolution, the TEM has become an all-in-one characterization tool. Indeed, most of the properties of a material can be directly mapped in the TEM, including the composition, structure, bonding, morphology, and defects. The scope of applications spans essentially all of the physical sciences and includes biology. Until recently, however, high resolution visualization of structural changes occurring on sub-millisecond time scales was not possible. In order to reach the ultrashort temporal domain within which fundamental atomic motions take place, while simultaneously retaining high spatial resolution, an entirely new approach from that of millisecond-limited TEM cameras had to be conceived. As shown below, the approach is also different from that of nanosecond-limited TEM, whose resolution cannot offer the ultrafast regimes of dynamics. For this reason "ultrafast electron microscopy" is reserved for the field which is concerned with femtosecond to picosecond resolution capability of structural dynamics. In conventional TEMs, electrons are produced by heating a source or by applying a strong extraction field. Both methods result in the stochastic emission of electrons, with no control over temporal spacing or relative arrival time at the specimen. The timing issue can be overcome by exploiting the photoelectric effect and using pulsed lasers to generate precisely timed electron packets of ultrashort duration. The spatial and temporal resolutions achievable with short intense pulses containing a large number of electrons, however, are limited to tens of nanometers and nanoseconds, respectively. This is because Coulomb repulsion is significant in such a pulse, and the electrons spread in space and time, thus limiting the beam coherence. It is therefore not possible to image the ultrafast elementary dynamics of complex transformations. The challenge was to retain the high spatial resolution of a conventional TEM while simultaneously enabling the temporal resolution required to visualize atomic-scale motions. In this Account, we discuss the development of four-dimensional ultrafast electron microscopy (4D UEM) and summarize techniques and applications that illustrate the power of the approach. In UEM, images are obtained either stroboscopically with coherent single-electron packets or with a single electron bunch. Coulomb repulsion is absent under the single-electron condition, thus permitting imaging, diffraction, and spectroscopy, all with high spatiotemporal resolution, the atomic scale (sub-nanometer and femtosecond). The time resolution is limited only by the laser pulse duration and energy carried by the electron packets; the CCD camera has no bearing on the temporal resolution. In the regime of single pulses of electrons, the temporal resolution of picoseconds can be attained when hundreds of electrons are in the bunch. The applications given here are selected to highlight phenomena of different length and time scales, from atomic motions during structural dynamics to phase transitions and nanomechanical oscillations. We conclude with a brief discussion of emerging methods, which include scanning ultrafast electron microscopy (S-UEM), scanning transmission ultrafast electron microscopy (ST-UEM) with convergent beams, and time-resolved imaging of biological structures at ambient conditions with environmental cells.

Biomechanical properties of the forefoot plantar soft tissue as measured by an optical coherence tomography-based air-jet indentation system and tissue ultrasound palpation system.

PubMed

Chao, Clare Y L; Zheng, Yong-Ping; Huang, Yan-Ping; Cheing, Gladys L Y

2010-07-01

The forefoot medial plantar area withstand high plantar pressure during locomotion, and is a common site that develops foot lesion problems among elderly people. The aims of the present study were to (1) determine the correlation between the biomechanical properties of forefoot medial plantar soft tissue measured by a newly developed optical coherence tomography-based air-jet indentation system and by tissue ultrasound palpation system, and (2) to compare the biomechanical properties of plantar soft tissues of medial forefoot between a young and old adult group. Thirty healthy subjects were classified as the young or older group. The biomechanical properties of plantar soft tissues measured at the forefoot by the air-jet indentation system and tissue ultrasound palpation system were performed, and the correlation of the findings obtained in the two systems were compared. A strong positive correlation was obtained from the findings in the two systems (r=0.88, P<0.001). The forefoot plantar soft tissue of the older group was significantly stiffer at the second metatarsal head and thinner at both metatarsal heads than that of the young group (all P<0.05). The stiffness coefficient at the second metatarsal head was 28% greater than that at the first metatarsal head in both study groups. Older subjects showed a loss of elasticity and reduced thickness in their forefoot plantar soft tissue, with the second metatarsal head displaying stiffer and thicker plantar tissue than the first metatarsal head. The air-jet indentation system is a useful instrument for characterizing the biomechanical properties of soft tissue. Copyright (c) 2010 Elsevier Ltd. All rights reserved.

Low Luminosity States of the Black Hole Candidate GX 339-4. 2; Timing Analysis

NASA Technical Reports Server (NTRS)

Nowak, Michael A.; Wilms, Joern; Dove, James B.

1999-01-01

Here we present timing analysis of a set of eight Rossi X-ray Timing Explorer (RXTE) observations of the black hole candidate GX 339-4 that were taken during its hard/low state. On long time scales, the RXTE All Sky Monitor data reveal evidence of a 240 day periodicity, comparable to timescales expected from warped, precessing accretion disks. On short timescales all observations save one show evidence of a persistent f(qpo approximately equals 0.3 Hz quasi-periodic oscillations (QPO)). The broad band (10 (exp -3) to 10 (exp2) Hz) power appears to be dominated by two independent processes that can be modeled as very broad Lorentzians with Q approximately less than - 1. The coherence function between soft and hard photon variability shows that if these are truly independent processes, then they are individually coherent, but they are incoherent with one another. This is evidenced by the fact that the coherence function between the hard and soft variability is near unity between 5 x 10 (exp -3) but shows evidence of a dip at f approximately equals 1 Hz. This is the region of overlap between the broad Lorentzian fits to the Power Spectral Density (PSD). Similar to Cyg X-1, the coherence also drops dramatically at frequencies approximately greater than 1O Hz. Also similar to Cyg X-1, the hard photon variability is seen to lag the soft photon variability with the lag time increasing with decreasing Fourier frequency. The magnitude of this time lag appears to be positively correlated with the flux of GX 339-4. We discuss all of these observations in light of current theoretical models of both black hole spectra and temporal variability.

Coherent soft X-ray high-order harmonics using tight-focusing laser pulses in the gas mixture.

PubMed

Lu, Faming; Xia, Yuanqin; Zhang, Sheng; Chen, Deying; Zhao, Yang; Liu, Bin

2014-01-01

We experimentally study the harmonics from a Xe-He gas mixture using tight-focusing femtosecond laser pulses. The spectrum in the mixed gases exhibits an extended cutoff region from the harmonic H21 to H27. The potential explanation is that the harmonics photons from Xe contribute the electrons of He atoms to transmit into the excited-state. Therefore, the harmonics are emitted from He atoms easily. Furthermore, we show that there are the suppressed harmonics H15 and H17 in the mixed gases. The underlying mechanism is the destructive interference between harmonics generated from different atoms. Our results indicate that HHG from Xe-He gas mixture is an efficient method of obtaining the coherent soft X-ray source.

Coherence properties of the radiation from FLASH

NASA Astrophysics Data System (ADS)

Schneidmiller, E. A.; Yurkov, M. V.

2016-02-01

Free electron LASer in Hamburg is the first free electron laser user facility operating in the vacuum ultraviolet and soft X-ray wavelength range. Many user experiments require knowledge of the spatial and temporal coherence properties of the radiation. In this paper, we present a theoretical analysis of the coherence properties of the radiation for the fundamental and for the higher odd frequency harmonics. We show that temporal and spatial coherence reach their maxima close to the free electron laser (FEL) saturation but may degrade significantly in the post-saturation regime. We also find that the pointing stability of short FEL pulses is limited due to the fact that nonazimuthal FEL eigenmodes are not sufficiently suppressed. We discuss possible ways for improving the degree of transverse coherence and the pointing stability.

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

Sissa, Cristina; Delchiaro, Francesca; Di Maiolo, Francesco

Essential-state models efficiently describe linear and nonlinear spectral properties of different families of charge-transfer chromophores. Here, the essential-state machinery is applied to the calculation of the early-stage dynamics after ultrafast (coherent) excitation of polar and quadrupolar chromophores. The fully non-adiabatic treatment of coupled electronic and vibrational motion allows for a reliable description of the dynamics of these intriguing systems. In particular, the proposed approach is reliable even when the adiabatic and harmonic approximations do not apply, such as for quadrupolar dyes that show a multistable, broken-symmetry excited state. Our approach quite naturally leads to a clear picture for a dynamicalmore » Jahn-Teller effect in these systems. The recovery of symmetry due to dynamical effects is however disrupted in polar solvents where a static symmetry lowering is observed. More generally, thermal disorder in polar solvents is responsible for dephasing phenomena, damping the coherent oscillations with particularly important effects in the case of polar dyes.« less

An exciton-polariton laser based on biologically produced fluorescent protein

PubMed Central

Dietrich, Christof P.; Steude, Anja; Tropf, Laura; Schubert, Marcel; Kronenberg, Nils M.; Ostermann, Kai; Höfling, Sven; Gather, Malte C.

2016-01-01

Under adequate conditions, cavity polaritons form a macroscopic coherent quantum state, known as polariton condensate. Compared to Wannier-Mott excitons in inorganic semiconductors, the localized Frenkel excitons in organic emitter materials show weaker interaction with each other but stronger coupling to light, which recently enabled the first realization of a polariton condensate at room temperature. However, this required ultrafast optical pumping, which limits the applications of organic polariton condensates. We demonstrate room temperature polariton condensates of cavity polaritons in simple laminated microcavities filled with biologically produced enhanced green fluorescent protein (eGFP). The unique molecular structure of eGFP prevents exciton annihilation even at high excitation densities, thus facilitating polariton condensation under conventional nanosecond pumping. Condensation is clearly evidenced by a distinct threshold, an interaction-induced blueshift of the condensate, long-range coherence, and the presence of a second threshold at higher excitation density that is associated with the onset of photon lasing. PMID:27551686

Real-space collapse of a polariton condensate

PubMed Central

Dominici, L.; Petrov, M.; Matuszewski, M.; Ballarini, D.; De Giorgi, M.; Colas, D.; Cancellieri, E.; Silva Fernández, B.; Bramati, A.; Gigli, G.; Kavokin, A.; Laussy, F.; Sanvitto, D.

2015-01-01

Microcavity polaritons are two-dimensional bosonic fluids with strong nonlinearities, composed of coupled photonic and electronic excitations. In their condensed form, they display quantum hydrodynamic features similar to atomic Bose–Einstein condensates, such as long-range coherence, superfluidity and quantized vorticity. Here we report the unique phenomenology that is observed when a pulse of light impacts the polariton vacuum: the fluid which is suddenly created does not splash but instead coheres into a very bright spot. The real-space collapse into a sharp peak is at odd with the repulsive interactions of polaritons and their positive mass, suggesting that an unconventional mechanism is at play. Our modelling devises a possible explanation in the self-trapping due to a local heating of the crystal lattice, that can be described as a collective polaron formed by a polariton condensate. These observations hint at the polariton fluid dynamics in conditions of extreme intensities and ultrafast times. PMID:26634817

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

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

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

2014-01-13

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

Davisson-Germer Prize in Atomic or Surface Physics Talk: Soft X-Ray Studies of Surfaces, Interfaces and Thin Films: From Spectroscopy to Ultrafast Nanoscale Movies

NASA Astrophysics Data System (ADS)

Stöhr, Joachim

2011-03-01

My talk will review the development of soft x-ray spectroscopy and microscopy and its impact on our understanding of chemical bonding, magnetism and dynamics at surfaces and interfaces. I will first outline important soft x-ray spectroscopy and microscopy techniques that have been developed over the last 30 years and their key strengths such as elemental and chemical specificity, sensitivity to small atomic concentrations, separation of charge and spin properties, spatial resolution down to the nanometer scale, and temporal resolution down to the intrinsic femtosecond timescale of atomic and electronic motions. I will then present scientific breakthroughs based on soft x-ray studies in three selected areas: the nature of molecular bonding and reactivity on metal surfaces, the molecular origin of liquid crystal alignment on surfaces, and the microscopic origin of interface-mediated spin alignments in modern magnetic devices. My talk will also cover the use of soft x-rays for revealing the temporal evolution of electronic structure, addressing the key problem of ``function,'' down to the intrinsic femtosecond time scale of charge and spin configuration changes. As examples I will present the formation and breaking of chemical bonds in surface complexes and the motion of the magnetization in magnetic devices. Work supported by the Office of Basic Energy Science of the US Department of Energy.

Optimal generation of spatially coherent soft X-ray isolated attosecond pulses in a gas-filled waveguide using two-color synthesized laser pulses

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

Jin, Cheng; Hong, Kyung -Han; Lin, C. D.

2016-12-08

Here, we numerically demonstrate the generation of intense, low-divergence soft X-ray isolated attosecond pulses in a gas-filled hollow waveguide using synthesized few-cycle two-color laser waveforms. The waveform is a superposition of a fundamental and its second harmonic optimized such that highest harmonic yields are emitted from each atom. We then optimize the gas pressure and the length and radius of the waveguide such that bright coherent high-order harmonics with angular divergence smaller than 1 mrad are generated, for photon energy from the extreme ultraviolet to soft X-rays. By selecting a proper spectral range enhanced isolated attosecond pulses are generated. Wemore » study how dynamic phase matching caused by the interplay among waveguide mode, neutral atomic dispersion, and plasma effect is achieved at the optimal macroscopic conditions, by performing time-frequency analysis and by analyzing the evolution of the driving laser’s electric field during the propagation. Our results, when combined with the on-going push of high-repetition-rate lasers (sub- to few MHz’s) may eventually lead to the generation of high-flux, low-divergence soft X-ray tabletop isolated attosecond pulses for applications.« less

Nonlinear dynamics and damage induced properties of soft matter with application in oncology

NASA Astrophysics Data System (ADS)

Naimark, O.

2017-09-01

Molecular-morphological signs of oncogenesis could be linked to multiscale collective effects in molecular, cell and tissue related to defects (damage) dynamics. It was shown that nonlinear behavior of biological systems can be linked to the existence of characteristic collective open state modes providing the coherent expression dynamics. New type of criticality in nonequilibrium systems with defects—structural-scaling transition allows the definition of the `driving force' for a biological soft matter related to consolidated open states. The set of collective open states (breathers, autosolitons and blow-up modes) in the molecular ensembles provides the collective expression dynamics to attract the entire system (cell, tissue) toward a few preferred global states. The co-existence of three types of collective modes determines the multifractal scenario of biological soft matter dynamics. The appearance of `globally convergent' dynamics corresponding to the coherent behavior of multiscale blow-up open states (blow-up gene expression) leads to anomalous localized softening (blow-up localized damage) and the subjection of the cells (or tissue) to monofractal dynamics. This dynamics can be associated with cancer progression.

Resonant acoustic spectroscopy of soft tissues using embedded magnetomotive nanotransducers and optical coherence tomography

PubMed Central

Oldenburg, Amy L

2010-01-01

We present a new method for performing dynamic elastography of soft tissue samples. By sensing nanoscale displacements with optical coherence tomography, a chirped, modulated force is applied to acquire the mechanical spectrum of a tissue sample within a few seconds. This modulated force is applied via magnetic nanoparticles, named ‘nanotransducers’, which are diffused into the tissue, and which contribute negligible inertia to the soft tissue mechanical system. Using this novel system, we observed that excised tissues exhibit mechanical resonance modes which are well described by a linear damped harmonic oscillator. Results are validated by using cylindrical tissue phantoms of agarose in which resonant frequencies (30–400 Hz) are consistent with longitudinal modes and the sample boundary conditions. We furthermore show that the Young’s modulus can be computed from their measured resonance frequencies, analogous to resonant ultrasound spectroscopy for stiff material analysis. Using this new technique, named magnetomotive resonant acoustic spectroscopy (MRAS), we monitored the relative stiffening of an excised rat liver during a chemical fixation process. PMID:20124653

Globally Stable Microresonator Turing Pattern Formation for Coherent High-Power THz Radiation On-Chip

NASA Astrophysics Data System (ADS)

Huang, Shu-Wei; Yang, Jinghui; Yang, Shang-Hua; Yu, Mingbin; Kwong, Dim-Lee; Zelevinsky, T.; Jarrahi, Mona; Wong, Chee Wei

2017-10-01

In nonlinear microresonators driven by continuous-wave (cw) lasers, Turing patterns have been studied in the formalism of the Lugiato-Lefever equation with emphasis on their high coherence and exceptional robustness against perturbations. Destabilization of Turing patterns and the transition to spatiotemporal chaos, however, limit the available energy carried in the Turing rolls and prevent further harvest of their high coherence and robustness to noise. Here, we report a novel scheme to circumvent such destabilization, by incorporating the effect of local mode hybridizations, and we attain globally stable Turing pattern formation in chip-scale nonlinear oscillators with significantly enlarged parameter space, achieving a record-high power-conversion efficiency of 45% and an elevated peak-to-valley contrast of 100. The stationary Turing pattern is discretely tunable across 430 GHz on a THz carrier, with a fractional frequency sideband nonuniformity measured at 7.3 ×10-14 . We demonstrate the simultaneous microwave and optical coherence of the Turing rolls at different evolution stages through ultrafast optical correlation techniques. The free-running Turing-roll coherence, 9 kHz in 200 ms and 160 kHz in 20 minutes, is transferred onto a plasmonic photomixer for one of the highest-power THz coherent generations at room temperature, with 1.1% optical-to-THz power conversion. Its long-term stability can be further improved by more than 2 orders of magnitude, reaching an Allan deviation of 6 ×10-10 at 100 s, with a simple computer-aided slow feedback control. The demonstrated on-chip coherent high-power Turing-THz system is promising to find applications in astrophysics, medical imaging, and wireless communications.

Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer.

PubMed

Duan, Hong-Guang; Prokhorenko, Valentyn I; Cogdell, Richard J; Ashraf, Khuram; Stevens, Amy L; Thorwart, Michael; Miller, R J Dwayne

2017-08-08

During the first steps of photosynthesis, the energy of impinging solar photons is transformed into electronic excitation energy of the light-harvesting biomolecular complexes. The subsequent energy transfer to the reaction center is commonly rationalized in terms of excitons moving on a grid of biomolecular chromophores on typical timescales [Formula: see text]100 fs. Today's understanding of the energy transfer includes the fact that the excitons are delocalized over a few neighboring sites, but the role of quantum coherence is considered as irrelevant for the transfer dynamics because it typically decays within a few tens of femtoseconds. This orthodox picture of incoherent energy transfer between clusters of a few pigments sharing delocalized excitons has been challenged by ultrafast optical spectroscopy experiments with the Fenna-Matthews-Olson protein, in which interference oscillatory signals up to 1.5 ps were reported and interpreted as direct evidence of exceptionally long-lived electronic quantum coherence. Here, we show that the optical 2D photon echo spectra of this complex at ambient temperature in aqueous solution do not provide evidence of any long-lived electronic quantum coherence, but confirm the orthodox view of rapidly decaying electronic quantum coherence on a timescale of 60 fs. Our results can be considered as generic and give no hint that electronic quantum coherence plays any biofunctional role in real photoactive biomolecular complexes. Because in this structurally well-defined protein the distances between bacteriochlorophylls are comparable to those of other light-harvesting complexes, we anticipate that this finding is general and directly applies to even larger photoactive biomolecular complexes.

Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer

NASA Astrophysics Data System (ADS)

Duan, Hong-Guang; Prokhorenko, Valentyn I.; Cogdell, Richard J.; Ashraf, Khuram; Stevens, Amy L.; Thorwart, Michael; Miller, R. J. Dwayne

2017-08-01

During the first steps of photosynthesis, the energy of impinging solar photons is transformed into electronic excitation energy of the light-harvesting biomolecular complexes. The subsequent energy transfer to the reaction center is commonly rationalized in terms of excitons moving on a grid of biomolecular chromophores on typical timescales <<100 fs. Today’s understanding of the energy transfer includes the fact that the excitons are delocalized over a few neighboring sites, but the role of quantum coherence is considered as irrelevant for the transfer dynamics because it typically decays within a few tens of femtoseconds. This orthodox picture of incoherent energy transfer between clusters of a few pigments sharing delocalized excitons has been challenged by ultrafast optical spectroscopy experiments with the Fenna-Matthews-Olson protein, in which interference oscillatory signals up to 1.5 ps were reported and interpreted as direct evidence of exceptionally long-lived electronic quantum coherence. Here, we show that the optical 2D photon echo spectra of this complex at ambient temperature in aqueous solution do not provide evidence of any long-lived electronic quantum coherence, but confirm the orthodox view of rapidly decaying electronic quantum coherence on a timescale of 60 fs. Our results can be considered as generic and give no hint that electronic quantum coherence plays any biofunctional role in real photoactive biomolecular complexes. Because in this structurally well-defined protein the distances between bacteriochlorophylls are comparable to those of other light-harvesting complexes, we anticipate that this finding is general and directly applies to even larger photoactive biomolecular complexes.

Experimental demonstration of a soft x-ray self-seeded free-electron laser.

PubMed

Ratner, D; Abela, R; Amann, J; Behrens, C; Bohler, D; Bouchard, G; Bostedt, C; Boyes, M; Chow, K; Cocco, D; Decker, F J; Ding, Y; Eckman, C; Emma, P; Fairley, D; Feng, Y; Field, C; Flechsig, U; Gassner, G; Hastings, J; Heimann, P; Huang, Z; Kelez, N; Krzywinski, J; Loos, H; Lutman, A; Marinelli, A; Marcus, G; Maxwell, T; Montanez, P; Moeller, S; Morton, D; Nuhn, H D; Rodes, N; Schlotter, W; Serkez, S; Stevens, T; Turner, J; Walz, D; Welch, J; Wu, J

2015-02-06

The Linac Coherent Light Source has added a self-seeding capability to the soft x-ray range using a grating monochromator system. We report the demonstration of soft x-ray self-seeding with a measured resolving power of 2000-5000, wavelength stability of 10(-4), and an increase in peak brightness by a factor of 2-5 across the photon energy range of 500-1000 eV. By avoiding the need for a monochromator at the experimental station, the self-seeded beam can deliver as much as 50-fold higher brightness to users.

longitudinal space charge assisted echo seeding of a free electron laser

NASA Astrophysics Data System (ADS)

Hacker, Kirsten

2015-05-01

Seed lasers are employed to improve the temporal coherence of free-electron laser light. However, when seed pulses are short relative to the particle bunch, the noisy, temporally incoherent radiation from the un-seeded electrons can overwhelm the coherent, seeded radiation. In this paper a new seeding mechanism to improve the contrast between coherent and incoherent free electron laser radiation is employed together with a novel, simplified echo-seeding method. The concept relies on a combination of longitudinal space charge wakes and an echo-seeding technique to make a short, coherent pulse of FEL light together with noise background suppression. Several different simulation codes are used to illustrate the concept with conditions at the soft x-ray Free-electron LASer in Hamburg, FLASH. The impacts of coherent synchrotron radiation, intra beam scattering, and high peak current operation are investigated.

Laser-based three-dimensional multiscale micropatterning of biocompatible hydrogels for customized tissue engineering scaffolds

PubMed Central

Applegate, Matthew B.; Coburn, Jeannine; Partlow, Benjamin P.; Moreau, Jodie E.; Mondia, Jessica P.; Marelli, Benedetto; Kaplan, David L.; Omenetto, Fiorenzo G.

2015-01-01

Light-induced material phase transitions enable the formation of shapes and patterns from the nano- to the macroscale. From lithographic techniques that enable high-density silicon circuit integration, to laser cutting and welding, light–matter interactions are pervasive in everyday materials fabrication and transformation. These noncontact patterning techniques are ideally suited to reshape soft materials of biological relevance. We present here the use of relatively low-energy (< 2 nJ) ultrafast laser pulses to generate 2D and 3D multiscale patterns in soft silk protein hydrogels without exogenous or chemical cross-linkers. We find that high-resolution features can be generated within bulk hydrogels through nearly 1 cm of material, which is 1.5 orders of magnitude deeper than other biocompatible materials. Examples illustrating the materials, results, and the performance of the machined geometries in vitro and in vivo are presented to demonstrate the versatility of the approach. PMID:26374842

Ultrafast Spectroscopy of Fano-Like Resonance between Optical Phonon and Excitons in CdSe Quantum Dots: Dependence of Coherent Vibrational Wave-Packet Dynamics on Pump Fluence

PubMed Central

Aybush, Arseniy; Gostev, Fedor; Shelaev, Ivan; Titov, Andrey; Umanskiy, Stanislav; Cherepanov, Dmitry

2017-01-01

The main goal of the present work is to study the coherent phonon in strongly confined CdSe quantum dots (QDs) under varied pump fluences. The main characteristics of coherent phonons (amplitude, frequency, phase, spectrogram) of CdSe QDs under the red-edge pump of the excitonic band [1S(e)-1S3/2(h)] are reported. We demonstrate for the first time that the amplitude of the coherent optical longitudinal-optical (LO) phonon at 6.16 THz excited in CdSe nanoparticles by a femtosecond unchirped pulse shows a non-monotone dependence on the pump fluence. This dependence exhibits the maximum at pump fluence ~0.8 mJ/cm2. At the same time, the amplitudes of the longitudinal acoustic (LA) phonon mode at 0.55 THz and of the coherent wave packet of toluene at 15.6, 23.6 THz show a monotonic rise with the increase of pump fluence. The time frequency representation of an oscillating signal corresponding to LO phonons revealed by continuous wavelet transform (CWT) shows a profound destructive quantum interference close to the origin of distinct (optical phonon) and continuum-like (exciton) quasiparticles. The CWT spectrogram demonstrates a nonlinear chirp at short time delays, where the chirp sign depends on the pump pulse fluence. The CWT spectrogram reveals an anharmonic coupling between optical and acoustic phonons. PMID:29113056

Ultrafast probes of nonequilibrium hole spin relaxation in the ferromagnetic semiconductor GaMnAs

NASA Astrophysics Data System (ADS)

Patz, Aaron; Li, Tianqi; Liu, Xinyu; Furdyna, Jacek K.; Perakis, Ilias E.; Wang, Jigang

2015-04-01

We report direct measurements of hole spin lifetimes in ferromagnetic GaMnAs carried out by time- and polarization-resolved spectroscopy. Below the Curie temperature, ultrafast photoexcitation of GaMnAs with linearly polarized light is shown to create a nonequilibrium hole spin population via dynamical polarization of the holes through p -d exchange scattering with ferromagnetically ordered Mn spins. The system is then observed to relax in a distinct three-step recovery process: (i) a femtosecond hole spin relaxation, on the scale of 160-200 fs; (ii) a picosecond hole energy relaxation, on the scale of 1-2 ps; and (iii) a coherent, damped Mn spin precession with a period of 250 ps. The transient amplitude of the hole spin relaxation component diminishes with increasing temperature, directly following the ferromagnetic order of GaMnAs, while the hole energy amplitude shows negligible temperature change. Our results serve to establish the hole spin lifetimes in the ferromagnetic semiconductor GaMnAs, at the same time demonstrating a spectroscopic method for studying nonequilibrium hole spins in the presence of magnetic order and spin-exchange interaction.

Quasicrystals and Quantum Computing

NASA Astrophysics Data System (ADS)

Berezin, Alexander A.

1997-03-01

In Quantum (Q) Computing qubits form Q-superpositions for macroscopic times. One scheme for ultra-fast (Q) computing can be based on quasicrystals. Ultrafast processing in Q-coherent structures (and the very existence of durable Q-superpositions) may be 'consequence' of presence of entire manifold of integer arithmetic (A0, aleph-naught of Georg Cantor) at any 4-point of space-time, furthermore, at any point of any multidimensional phase space of (any) N-particle Q-system. The latter, apart from quasicrystals, can include dispersed and/or diluted systems (Berezin, 1994). In such systems such alleged centrepieces of Q-Computing as ability for fast factorization of long integers can be processed by sheer virtue of the fact that entire infinite pattern of prime numbers is instantaneously available as 'free lunch' at any instant/point. Infinitely rich pattern of A0 (including pattern of primes and almost primes) acts as 'independent' physical effect which directly generates Q-dynamics (and physical world) 'out of nothing'. Thus Q-nonlocality can be ultimately based on instantaneous interconnectedness through ever- the-same structure of A0 ('Platonic field' of integers).

Ultrafast Three-Dimensional Integrated Imaging of Strain in Core/Shell Semiconductor/Metal Nanostructures

DOE PAGES

Cherukara, Mathew J.; Sasikumar, Kiran; DiChiara, Anthony; ...

2017-11-07

Visualizing the dynamical response of material heterointerfaces is increasingly important for the design of hybrid materials and structures with tailored properties for use in functional devices. In situ characterization of nanoscale heterointerfaces such as metal-semiconductor interfaces, which exhibit a complex interplay between lattice strain, electric potential, and heat transport at subnanosecond time scales, is particularly challenging. Here in this work, we use a laser pump/X-ray probe form of Bragg coherent diffraction imaging (BCDI) to visualize in three-dimension the deformation of the core of a model core/shell semiconductor-metal (ZnO/Ni) nanorod following laser heating of the shell. We observe a rich interplaymore » of radial, axial, and shear deformation modes acting at different time scales that are induced by the strain from the Ni shell. We construct experimentally informed models by directly importing the reconstructed crystal from the ultrafast experiment into a thermo-electromechanical continuum model. The model elucidates the origin of the deformation modes observed experimentally. Our integrated imaging approach represents an invaluable tool to probe strain dynamics across mixed interfaces under operando conditions.« less

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Theory of low-power ultra-broadband terahertz sideband generation in bi-layer graphene

PubMed Central

Crosse, J. A.; Xu, Xiaodong; Sherwin, Mark S.; Liu, R. B.

2014-01-01

In a semiconductor illuminated by a strong terahertz (THz) field, optically excited electron–hole pairs can recombine to emit light in a broad frequency comb evenly spaced by twice the THz frequency. Such high-order THz sideband generation is of interest both as an example of extreme nonlinear optics and also as a method for ultrafast electro-optical modulation. So far, this phenomenon has only been observed with large field strengths (~10 kV cm−1), an obstacle for technological applications. Here we predict that bi-layer graphene generates high-order sidebands at much weaker THz fields. We find that a THz field of strength 1 kV cm−1 can produce a high-sideband spectrum of about 30 THz, 100 times broader than in GaAs. The sidebands are generated despite the absence of classical collisions, with the quantum coherence of the electron–hole pairs enabling recombination. These remarkable features lower the barrier to desktop electro-optical modulation at THz frequencies, facilitating ultrafast optical communications. PMID:25249245

Imaging nanoscale spatial modulation of a relativistic electron beam with a MeV ultrafast electron microscope

NASA Astrophysics Data System (ADS)

Lu, Chao; Jiang, Tao; Liu, Shengguang; Wang, Rui; Zhao, Lingrong; Zhu, Pengfei; Liu, Yaqi; Xu, Jun; Yu, Dapeng; Wan, Weishi; Zhu, Yimei; Xiang, Dao; Zhang, Jie

2018-03-01

An accelerator-based MeV ultrafast electron microscope (MUEM) has been proposed as a promising tool to the study structural dynamics at the nanometer spatial scale and the picosecond temporal scale. Here, we report experimental tests of a prototype MUEM where high quality images with nanoscale fine structures were recorded with a pulsed ˜3 MeV picosecond electron beam. The temporal and spatial resolutions of the MUEM operating in the single-shot mode are about 4 ps (FWHM) and 100 nm (FWHM), corresponding to a temporal-spatial resolution of 4 × 10-19 s m, about 2 orders of magnitude higher than that achieved with state-of-the-art single-shot keV UEM. Using this instrument, we offer the demonstration of visualizing the nanoscale periodic spatial modulation of an electron beam, which may be converted into longitudinal density modulation through emittance exchange to enable production of high-power coherent radiation at short wavelengths. Our results mark a great step towards single-shot nanometer-resolution MUEMs and compact intense x-ray sources that may have widespread applications in many areas of science.

Measurement of high-dynamic range x-ray Thomson scattering spectra for the characterization of nano-plasmas at LCLS

DOE PAGES

MacDonald, M. J.; Gorkhover, T.; Bachmann, B.; ...

2016-08-08

Atomic clusters can serve as ideal model systems for exploring ultrafast (~100 fs) laser-driven ionization dynamics of dense matter on the nanometer scale. Resonant absorption of optical laser pulses enables heating to temperatures on the order of 1 keV at near solid density conditions. To date, direct probing of transient states of such nano plasmas was limited to coherent x-ray imaging. Here we present the first measurement of spectrally-resolved incoherent x-ray scattering from clusters, enabling measurements of transient temperature, densities and ionization. Single shot x-ray Thomson scatterings signals were recorded at 120 Hz using a crystal spectrometer in combination withmore » a single-photon counting and energy-dispersive pnCCD. A precise pump laser collimation scheme enabled recording near background-free scattering spectra from Ar clusters with an unprecedented dynamic range of more than 3 orders of magnitude. As a result, such measurements are important for understanding collective effects in laser-matter interactions on femtosecond timescales, opening new routes for the development of schemes for their ultrafast control.« less

Ultrafast Three-Dimensional Integrated Imaging of Strain in Core/Shell Semiconductor/Metal Nanostructures

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

Cherukara, Mathew J.; Sasikumar, Kiran; DiChiara, Anthony

Visualizing the dynamical response of material heterointerfaces is increasingly important for the design of hybrid materials and structures with tailored properties for use in functional devices. In situ characterization of nanoscale heterointerfaces such as metal-semiconductor interfaces, which exhibit a complex interplay between lattice strain, electric potential, and heat transport at subnanosecond time scales, is particularly challenging. Here in this work, we use a laser pump/X-ray probe form of Bragg coherent diffraction imaging (BCDI) to visualize in three-dimension the deformation of the core of a model core/shell semiconductor-metal (ZnO/Ni) nanorod following laser heating of the shell. We observe a rich interplaymore » of radial, axial, and shear deformation modes acting at different time scales that are induced by the strain from the Ni shell. We construct experimentally informed models by directly importing the reconstructed crystal from the ultrafast experiment into a thermo-electromechanical continuum model. The model elucidates the origin of the deformation modes observed experimentally. Our integrated imaging approach represents an invaluable tool to probe strain dynamics across mixed interfaces under operando conditions.« less

Measurement of high-dynamic range x-ray Thomson scattering spectra for the characterization of nano-plasmas at LCLS

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

MacDonald, M. J., E-mail: macdonm@umich.edu; SLAC National Accelerator Laboratory, Menlo Park, California 94025; Gorkhover, T.

2016-11-15

Atomic clusters can serve as ideal model systems for exploring ultrafast (∼100 fs) laser-driven ionization dynamics of dense matter on the nanometer scale. Resonant absorption of optical laser pulses enables heating to temperatures on the order of 1 keV at near solid density conditions. To date, direct probing of transient states of such nano-plasmas was limited to coherent x-ray imaging. Here we present the first measurement of spectrally resolved incoherent x-ray scattering from clusters, enabling measurements of transient temperature, densities, and ionization. Single shot x-ray Thomson scattering signals were recorded at 120 Hz using a crystal spectrometer in combination withmore » a single-photon counting and energy-dispersive pnCCD. A precise pump laser collimation scheme enabled recording near background-free scattering spectra from Ar clusters with an unprecedented dynamic range of more than 3 orders of magnitude. Such measurements are important for understanding collective effects in laser-matter interactions on femtosecond time scales, opening new routes for the development of schemes for their ultrafast control.« less

Ultrafast Three-Dimensional Integrated Imaging of Strain in Core/Shell Semiconductor/Metal Nanostructures.

PubMed

Cherukara, Mathew J; Sasikumar, Kiran; DiChiara, Anthony; Leake, Steven J; Cha, Wonsuk; Dufresne, Eric M; Peterka, Tom; McNulty, Ian; Walko, Donald A; Wen, Haidan; Sankaranarayanan, Subramanian K R S; Harder, Ross J

2017-12-13

Visualizing the dynamical response of material heterointerfaces is increasingly important for the design of hybrid materials and structures with tailored properties for use in functional devices. In situ characterization of nanoscale heterointerfaces such as metal-semiconductor interfaces, which exhibit a complex interplay between lattice strain, electric potential, and heat transport at subnanosecond time scales, is particularly challenging. In this work, we use a laser pump/X-ray probe form of Bragg coherent diffraction imaging (BCDI) to visualize in three-dimension the deformation of the core of a model core/shell semiconductor-metal (ZnO/Ni) nanorod following laser heating of the shell. We observe a rich interplay of radial, axial, and shear deformation modes acting at different time scales that are induced by the strain from the Ni shell. We construct experimentally informed models by directly importing the reconstructed crystal from the ultrafast experiment into a thermo-electromechanical continuum model. The model elucidates the origin of the deformation modes observed experimentally. Our integrated imaging approach represents an invaluable tool to probe strain dynamics across mixed interfaces under operando conditions.

Triplet exciton dissociation and electron extraction in graphene-templated pentacene observed with ultrafast spectroscopy.

PubMed

McDonough, Thomas J; Zhang, Lushuai; Roy, Susmit Singha; Kearns, Nicholas M; Arnold, Michael S; Zanni, Martin T; Andrew, Trisha L

2017-02-08

We compare the ultrafast dynamics of singlet fission and charge generation in pentacene films grown on glass and graphene. Pentacene grown on graphene is interesting because it forms large crystals with the long axis of the molecules "lying-down" (parallel to the surface). At low excitation fluence, spectra for pentacene on graphene contain triplet absorptions at 507 and 545 nm and no bleaching at 630 nm, which we show is due to the orientation of the pentacene molecules. We perform the first transient absorption anisotropy measurements on pentacene, observing negative anisotropy of the 507 and 545 nm peaks, consistent with triplet absorption. A broad feature at 853 nm, observed on both glass and graphene, is isotropic, suggesting hole absorption. At high fluence, there are additional features, whose kinetics and anisotropies are not explained by heating, that we assign to charge generation; we propose a polaron pair absorption at 614 nm. The lifetimes are shorter at high fluence for both pentacene on glass and graphene, indicative of triplet-triplet annihilation that likely enhances charge generation. The anisotropy decays more slowly for pentacene on graphene than on glass, in keeping with the smaller domain size observed via atomic force microscopy. Coherent acoustic phonons are observed for pentacene on graphene, which is a consequence of more homogeneous domains. Measuring the ultrafast dynamics of pentacene as a function of molecular orientation, fluence, and polarization provides new insight to previous spectral assignments.

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

PubMed

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

2011-03-01

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

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

PubMed Central

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

2011-01-01

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

Exciton-polariton dynamics in a GaAs bulk microcavity

NASA Astrophysics Data System (ADS)

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

1998-01-01

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

Energy Transfer Between Coherently Delocalized States in Thin Films of the Explosive Pentaerythritol Tetranitrate (PETN) Revealed by Two-Dimensional Infrared Spectroscopy

NASA Astrophysics Data System (ADS)

Ostrander, Joshua; Knepper, Robert; Tappan, Alexander; Kay, Jeffery; Zanni, Martin; Farrow, Darcie

2017-06-01

Pentaerythritol tetranitrate (PETN) is a common secondary explosive and has been used extensively to study shock initiation and energy propagation in energetic materials. We report 2D IR measurements of PETN thin films that resolve vibrational energy transfer and relaxation mechanisms. Ultrafast anisotropy measurements reveal a sub-500 fs reorientation of transition dipoles in thin films of vapor-deposited PETN that is absent in solution measurements, consistent with intermolecular energy transfer. The anisotropy is frequency dependent, suggesting spectrally heterogeneous vibrational relaxation. Cross peaks are observed in 2D IR spectra that resolve a specific energy transfer pathway with a 2 ps time scale. Measurements of the transition dipole strength indicate that these vibrational modes are coherently delocalized over at least 15-30 molecules. We discuss the implications of vibrational relaxation between coherently delocalized eigenstates for mechanisms relevant to explosives. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

Arbitrarily shaped high-coherence electron bunches from cold atoms

NASA Astrophysics Data System (ADS)

McCulloch, A. J.; Sheludko, D. V.; Saliba, S. D.; Bell, S. C.; Junker, M.; Nugent, K. A.; Scholten, R. E.

2011-10-01

Ultrafast electron diffractive imaging of nanoscale objects such as biological molecules and defects in solid-state devices provides crucial information on structure and dynamic processes: for example, determination of the form and function of membrane proteins, vital for many key goals in modern biological science, including rational drug design. High brightness and high coherence are required to achieve the necessary spatial and temporal resolution, but have been limited by the thermal nature of conventional electron sources and by divergence due to repulsive interactions between the electrons, known as the Coulomb explosion. It has been shown that, if the electrons are shaped into ellipsoidal bunches with uniform density, the Coulomb explosion can be reversed using conventional optics, to deliver the maximum possible brightness at the target. Here we demonstrate arbitrary and real-time control of the shape of cold electron bunches extracted from laser-cooled atoms. The ability to dynamically shape the electron source itself and to observe this shape in the propagated electron bunch provides a remarkable experimental demonstration of the intrinsically high spatial coherence of a cold-atom electron source, and the potential for alleviation of electron-source brightness limitations due to Coulomb explosion.

The birth of a quasiparticle in silicon observed in time-frequency space.

PubMed

Hase, Muneaki; Kitajima, Masahiro; Constantinescu, Anca Monia; Petek, Hrvoje

2003-11-06

The concept of quasiparticles in solid-state physics is an extremely powerful tool for describing complex many-body phenomena in terms of single-particle excitations. Introducing a simple particle, such as an electron, hole or phonon, deforms a many-body system through its interactions with other particles. In this way, the added particle is 'dressed' or 'renormalized' by a self-energy cloud that describes the response of the many-body system, so forming a new entity--the quasiparticle. Using ultrafast laser techniques, it is possible to impulsively generate bare particles and observe their subsequent dressing by the many-body interactions (that is, quasiparticle formation) on the time and energy scales governed by the Heisenberg uncertainty principle. Here we describe the coherent response of silicon to excitation with a 10-femtosecond (10(-14) s) laser pulse. The optical pulse interacts with the sample by way of the complex second-order nonlinear susceptibility to generate a force on the lattice driving coherent phonon excitation. Transforming the transient reflectivity signal into frequency-time space reveals interference effects leading to the coherent phonon generation and subsequent dressing of the phonon by electron-hole pair excitations.

Strong influence of coadsorbate interaction on CO desorption dynamics on Ru(0001) probed by ultrafast x-ray spectroscopy and ab initio simulations

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

Xin, H.; LaRue, J.; Oberg, H.

2015-04-16

We show that coadsorbed oxygen atoms have a dramatic influence on the CO desorption dynamics from Ru(0001). In contrast to the precursor-mediated desorption mechanism on Ru(0001), the presence of surface oxygen modifies the electronic structure of Ru atoms such that CO desorption occurs predominantly via the direct pathway. This phenomenon is directly observed in an ultrafast pump-probe experiment using a soft x-ray free-electron laser to monitor the dynamic evolution of the valence electronic structure of the surface species. This is supported with the potential of mean force along the CO desorption path obtained from density-functional theory calculations. Charge density distributionmore » and frozen-orbital analysis suggest that the oxygen-induced reduction of the Pauli repulsion, and consequent increase of the dative interaction between the CO 5σ and the charged Ru atom, is the electronic origin of the distinct desorption dynamics. Ab initio molecular dynamics simulations of CO desorption from Ru(0001) and oxygen-coadsorbed Ru(0001) provide further insights into the surface bond-breaking process.« less

An optical coherence tomography (OCT)-based air jet indentation system for measuring the mechanical properties of soft tissues

PubMed Central

Huang, Yan-Ping; Zheng, Yong-Ping; Wang, Shu-Zhe; Chen, Zhong-Ping; Huang, Qing-Hua; He, Yong-Hong

2010-01-01

A novel noncontact indentation system with the combination of an air jet and optical coherence tomography (OCT) was presented in this paper for the quantitative measurement of the mechanical properties of soft tissues. The key idea of this method is to use a pressure-controlled air jet as an indenter to compress the soft tissue in a noncontact way and utilize the OCT signals to extract the deformation induced. This indentation system provides measurement and mapping of tissue elasticity for small specimens with high scanning speed. Experiments were performed on 27 silicone tissue-mimicking phantoms with different Young’s moduli, which were also measured by uniaxial compression tests. The regression coefficient of the indentation force to the indentation depth (N mm−1) was used as an indicator of the stiffness of tissue under air jet indentation. Results showed that the stiffness coefficients measured by the current system correlated well with the corresponding Young’s moduli obtained by conventional mechanical testing (r = 0.89, p < 0.001). Preliminary in vivo tests also showed that the change of soft tissue stiffness with and without the contraction of the underlying muscles in the hand could be differentiated by the current measurement. This system may have broad applications in tissue assessment and characterization where alterations of mechanical properties are involved, in particular with the potential of noncontact micro-indentation for tissues. PMID:20463843

Cross polarization optical coherence tomography for diagnosis of oral soft tissues

NASA Astrophysics Data System (ADS)

Gladkova, Natalia; Karabut, Maria; Kiseleva, Elena; Robakidze, Natalia; Muraev, Alexander; Fomina, Julia

2011-03-01

We consider the capabilities of cross-polarization OCT (CP OCT) focused on comparison of images resulting from cross-polarization and co-polarization scattering simultaneously for diagnosis of oral soft tissues. CP OCT was done for 35 patients with dental implants and 30 patients with inflammatory intestine diseases. Our study showed good diagnostic capabilities of CP OCT for detecting soft tissue pathology in the oral cavity. The cross-polarized images demonstrate the ability of tissue to depolarize. CP OCT demonstrates clinical capabilities for early diagnosis of inflammatory intestine diseases by the state of oral cavity mucosa and for early detection of gingivitis in patients above implant.

Laser-speckle-visibility acoustic spectroscopy in soft turbid media.

PubMed

Wintzenrieth, Frédéric; Cohen-Addad, Sylvie; Le Merrer, Marie; Höhler, Reinhard

2014-01-01

We image the evolution in space and time of an acoustic wave propagating along the surface of turbid soft matter by shining coherent light on the sample. The wave locally modulates the speckle interference pattern of the backscattered light, which is recorded using a camera. We show both experimentally and theoretically how the temporal and spatial correlations in this pattern can be analyzed to obtain the acoustic wavelength and attenuation length. The technique is validated using shear waves propagating in aqueous foam. It may be applied to other kinds of acoustic waves in different forms of turbid soft matter such as biological tissues, pastes, or concentrated emulsions.

Laser-speckle-visibility acoustic spectroscopy in soft turbid media

NASA Astrophysics Data System (ADS)

Wintzenrieth, Frédéric; Cohen-Addad, Sylvie; Le Merrer, Marie; Höhler, Reinhard

2014-01-01

We image the evolution in space and time of an acoustic wave propagating along the surface of turbid soft matter by shining coherent light on the sample. The wave locally modulates the speckle interference pattern of the backscattered light, which is recorded using a camera. We show both experimentally and theoretically how the temporal and spatial correlations in this pattern can be analyzed to obtain the acoustic wavelength and attenuation length. The technique is validated using shear waves propagating in aqueous foam. It may be applied to other kinds of acoustic waves in different forms of turbid soft matter such as biological tissues, pastes, or concentrated emulsions.

Development of an adaptable coherent x-ray diffraction microscope with the emphasis on imaging hydrated specimens.

PubMed

Nam, Daewoong; Park, Jaehyun; Gallagher-Jones, Marcus; Shimada, Hiroki; Kim, Sangsoo; Kim, Sunam; Kohmura, Yoshiki; Ishikawa, Tetsuya; Song, Changyong

2013-11-01

This paper describes the development of a versatile coherent x-ray diffraction microscope capable of imaging biological specimens in solution. The microscope is a flexible platform accommodating various conditions, from low vacuum (10(-2) Pa) to helium gas filled ambient pressure. This flexibility greatly expands the application area, from in situ materials science to biology systems in their native state, by significantly relaxing restrictions to the sample environment. The coherent diffraction microscope has been used successfully to image a yeast cell immersed in buffer solution. We believe that the design of this coherent diffraction microscope can be directly adapted to various platforms such as table top soft x-ray laser, synchrotron x-ray sources, and x-ray free electron laser with minor relevant adjustments.

Development of an adaptable coherent x-ray diffraction microscope with the emphasis on imaging hydrated specimens

NASA Astrophysics Data System (ADS)

Nam, Daewoong; Park, Jaehyun; Gallagher-Jones, Marcus; Shimada, Hiroki; Kim, Sangsoo; Kim, Sunam; Kohmura, Yoshiki; Ishikawa, Tetsuya; Song, Changyong

2013-11-01

This paper describes the development of a versatile coherent x-ray diffraction microscope capable of imaging biological specimens in solution. The microscope is a flexible platform accommodating various conditions, from low vacuum (10-2 Pa) to helium gas filled ambient pressure. This flexibility greatly expands the application area, from in situ materials science to biology systems in their native state, by significantly relaxing restrictions to the sample environment. The coherent diffraction microscope has been used successfully to image a yeast cell immersed in buffer solution. We believe that the design of this coherent diffraction microscope can be directly adapted to various platforms such as table top soft x-ray laser, synchrotron x-ray sources, and x-ray free electron laser with minor relevant adjustments.

Characterization of Soft Contact Lens Edge Fitting during Daily Wear Using Ultrahigh-Resolution Optical Coherence Tomography.

PubMed

Cui, Lele; Chen, Sisi; Zhou, Weihe; Sheng, Kaixuan; Zhang, Lei; Shen, Meixiao; Li, Ming

2018-01-01

To determine conjunctival overlap over the edge of soft contact lens and to visualize the peripheral postlens tear film (PoLTF) underneath soft contact lenses using ultrahigh-resolution optical coherence tomography (UHR-OCT). Twenty participants (4 males and 16 females, 23.0 ± 3.7 years) were fitted with two different types of soft contact lenses randomly. The limbus with lens was imaged with the UHR-OCT at the horizontal meridian every two hours up to 6 hours during lens wear. The conjunctival overlap was ranked as the percentage of the edge covered by the conjunctiva. The frequency of occurrence for visualized peripheral PoLTF was determined. The average conjunctival overlaps at insertion were 49% and 73% for galyfilcon A and balafilcon A lenses and increased significantly to 84% and 90% by 6 hours of lens wear ( P < 0.001). Lenses with rounded edges had more conjunctival overlap than the lenses with angled edges ( P =0.014). There were significant decreases for PoLTF on the conjunctiva ( P =0.014) and peripheral cornea ( P =0.004) over the study period compared to insertion. The percentage of subjects with PoLTF on the conjunctiva (32.5%) and peripheral cornea (36%) were greater in subjects wearing balafilcon A lenses ( P =0.017). Increased conjunctival overlap over the lens edges and reduced PoLTF underneath the peripheral region of soft contact lenses were shown during lens daily wear. The lens edge configuration may play a role in conjunctival response and peripheral PoLTF.

Ultrafast studies of gold, nickel, and palladium nanorods

NASA Astrophysics Data System (ADS)

Sando, Gerald M.; Berry, Alan D.; Owrutsky, Jeffrey C.

2007-08-01

Steady state and ultrafast transient absorption studies have been carried out for gold, nickel, and palladium high aspect ratio nanorods. For each metal, nanorods were fabricated by electrochemical deposition into ˜6μm thick polycarbonate templates. Two nominal pore diameters(10 and 30nm, resulting in nanorod diameters of about 40 and 60nm, respectively) were used, yielding nanorods with high aspect ratios (>25). Static spectra of nanorods of all three metals reveal both a longitudinal surface plasmon resonance (SPRL) band in the mid-infrared as well as a transverse band in the visible for the gold and larger diameter nickel and palladium nanorods. The appearance of SPRL bands in the infrared for high aspect ratio metal nanorods and the trends in their maxima for the different aspect ratios and metals are consistent with calculations based on the Gans theory. For the gold and nickel samples, time resolved studies were performed with a subpicosecond resolution using 400nm excitation and a wide range of probe wavelengths from the visible to the mid-IR as well as for infrared excitation (near 2000cm-1) probed at 800nm. The dynamics observed for nanorods of both metals and both diameters include transients due to electron-phonon coupling and impulsively excited coherent acoustic breathing mode oscillations, which are similar to those previously reported for spherical and smaller rod-shaped gold nanoparticles. The dynamics we observe are the same within the experimental uncertainty for 400nm and infrared (5μm) excitation probed at 800nm. The transient absorption using 400nm excitation and 800nm probe pulses of the palladium nanorods also reveal coherent acoustic oscillations. The results demonstrate that the dynamics for high aspect ratio metal nanorods are similar to those for smaller nanoparticles.

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.

In vivo imaging in the oral cavity by endoscopic optical coherence tomography.

PubMed

Walther, Julia; Schnabel, Christian; Tetschke, Florian; Rosenauer, Tobias; Golde, Jonas; Ebert, Nadja; Baumann, Michael; Hannig, Christian; Koch, Edmund

2018-03-01

The common way to diagnose hard and soft tissue irregularities in the oral cavity is initially the visual inspection by an experienced dentist followed by further medical examinations, such as radiological imaging and/or histopathological investigation. For the diagnosis of oral hard and soft tissues, the detection of early transformations is mostly hampered by poor visual access, low specificity of the diagnosis techniques, and/or limited feasibility of frequent screenings. Therefore, optical noninvasive diagnosis of oral tissue is promising to improve the accuracy of oral screening. Considering this demand, a rigid handheld endoscopic scanner was developed for optical coherence tomography (OCT). The novelty is the usage of a commercially near-infrared endoscope with fitting optics in combination with an established spectral-domain OCT system of our workgroup. By reaching a high spatial resolution, in vivo images of anterior and especially posterior dental and mucosal tissues were obtained from the oral cavity of two volunteers. The convincing image quality of the endoscopic OCT device is particularly obvious for the imaging of different regions of the human soft palate with highly scattering fibrous layer and capillary network within the lamina propria. (2018) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE).

Nanometer-scale ablation using focused, coherent extreme ultraviolet/soft x-ray light

DOEpatents

Menoni, Carmen S [Fort Collins, CO; Rocca, Jorge J [Fort Collins, CO; Vaschenko, Georgiy [San Diego, CA; Bloom, Scott [Encinitas, CA; Anderson, Erik H [El Cerrito, CA; Chao, Weilun [El Cerrito, CA; Hemberg, Oscar [Stockholm, SE

2011-04-26

Ablation of holes having diameters as small as 82 nm and having clean walls was obtained in a poly(methyl methacrylate) on a silicon substrate by focusing pulses from a Ne-like Ar, 46.9 nm wavelength, capillary-discharge laser using a freestanding Fresnel zone plate diffracting into third order is described. Spectroscopic analysis of light from the ablation has also been performed. These results demonstrate the use of focused coherent EUV/SXR light for the direct nanoscale patterning of materials.

Phase-matched generation of coherent soft and hard X-rays using IR lasers

DOEpatents

Popmintchev, Tenio V.; Chen, Ming-Chang; Bahabad, Alon; Murnane, Margaret M.; Kapteyn, Henry C.

2013-06-11

Phase-matched high-order harmonic generation of soft and hard X-rays is accomplished using infrared driving lasers in a high-pressure non-linear medium. The pressure of the non-linear medium is increased to multi-atmospheres and a mid-IR (or higher) laser device provides the driving pulse. Based on this scaling, also a general method for global optimization of the flux of phase-matched high-order harmonic generation at a desired wavelength is designed.

Preliminary studies of radiation coupling between remote soft X-ray laser amplifiers

NASA Astrophysics Data System (ADS)

Cairns, G.; Lewis, C. L. S.; Macphee, A. G.; Neely, D.; Holden, M.; Krishnan, J.; Tallents, G. J.; Key, M. H.; Norreys, P. N.; Smith, C. G.; Zhang, J.; Holden, P. B.; Pert, G. J.; Plowes, J.; Ramsden, S. A.

1994-01-01

Coupling of a soft X-ray laser beam with a relaying concave mirror in a sequentially pumped amplifier geometry using the Ne-like Ge system has been studied experimentally. Preliminary observations indicate an increase in the spatial coherence of the amplified relayed beam. In addition, near-field imaging of one of the amplifier plasmas shows a double-lobed intensity pattern of the emergent beam indicating refractive guiding of the amplified beam with components both normal and tangential to the target surface.

The Dawn of Ultrafast Nonlinear Optics in the Terahertz Regime

NASA Astrophysics Data System (ADS)

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

The terahertz (THz) frequency range is a specific region of the electromagnetic spectrum also known as the far-infrared (FIR) region. More precisely, THz waves cover the region from 100 GHz to 20 THz, thus bridging the gap between microwaves and infrared light. Physically, 1 THz is equivalent to a wavelength of 300 μm in vacuum, to 33.3 cm-1 in terms of wave numbers, to a photon energy of 4 meV, or to a temperature of 48 K. THz waves have the ability to penetrate various materials including non-metallic compounds (papers and plastics), organics, gases, and liquids, thus being a powerful tool for spectroscopic sensing [1]. This portion of the electromagnetic spectrum has been accessible for some time by various means including molecular gas lasers, gyrotrons, and free-electron lasers [2]. Due to complexity, cost, and limited frequencies of operation, these sources have traditionally made it difficult to gain full access to the terahertz frequency range. Nevertheless, there were several pioneering works in nonlinear FIR spectroscopy already in the early 1970s, about one decade after the advent of the laser (readers may find a review in [3]). In particular, saturated absorption in the FIR region was first studied in 1970, which led to the optically pumped FIR gas laser [4]. In the 1980s, the first demonstration of THz radiation coherently generated and detected was made. This result coincided with the development of ultrafast lasers and was obtained using a photoconductive antenna emitter [5], where photoexcited carriers induced by an ultrafast laser pulse are accelerated by a biasing electric field. The resulting time varying current J(t) radiates an electromagnetic transient, E ∝ partial J/partial t , whose amplitude and phase depend on various parameters such as carrier mobility, carrier lifetime, bias field, and on the impurity doping concentration [6]. This allowed the birth of coherent time-domain THz spectroscopy (TDTS) [1], which provided unprecedented insights into the nature of molecular vibrations, carrier dynamics in semiconductors, and protein kinetics [7-12]. Even with 30 years of rapid advances in the study of light-matter interactions at THz frequencies, lack of efficient emitters and sensitive detectors in this frequency range has for long time slowed down THz linear and nonlinear spectroscopy.

AXSIS: Exploring the frontiers in attosecond X-ray science, imaging and spectroscopy.

PubMed

Kärtner, F X; Ahr, F; Calendron, A-L; Çankaya, H; Carbajo, S; Chang, G; Cirmi, G; Dörner, K; Dorda, U; Fallahi, A; Hartin, A; Hemmer, M; Hobbs, R; Hua, Y; Huang, W R; Letrun, R; Matlis, N; Mazalova, V; Mücke, O D; Nanni, E; Putnam, W; Ravi, K; Reichert, F; Sarrou, I; Wu, X; Yahaghi, A; Ye, H; Zapata, L; Zhang, D; Zhou, C; Miller, R J D; Berggren, K K; Graafsma, H; Meents, A; Assmann, R W; Chapman, H N; Fromme, P

2016-09-01

X-ray crystallography is one of the main methods to determine atomic-resolution 3D images of the whole spectrum of molecules ranging from small inorganic clusters to large protein complexes consisting of hundred-thousands of atoms that constitute the macromolecular machinery of life. Life is not static, and unravelling the structure and dynamics of the most important reactions in chemistry and biology is essential to uncover their mechanism. Many of these reactions, including photosynthesis which drives our biosphere, are light induced and occur on ultrafast timescales. These have been studied with high time resolution primarily by optical spectroscopy, enabled by ultrafast laser technology, but they reduce the vast complexity of the process to a few reaction coordinates. In the AXSIS project at CFEL in Hamburg, funded by the European Research Council, we develop the new method of attosecond serial X-ray crystallography and spectroscopy, to give a full description of ultrafast processes atomically resolved in real space and on the electronic energy landscape, from co-measurement of X-ray and optical spectra, and X-ray diffraction. This technique will revolutionize our understanding of structure and function at the atomic and molecular level and thereby unravel fundamental processes in chemistry and biology like energy conversion processes. For that purpose, we develop a compact, fully coherent, THz-driven atto-second X-ray source based on coherent inverse Compton scattering off a free-electron crystal, to outrun radiation damage effects due to the necessary high X-ray irradiance required to acquire diffraction signals. This highly synergistic project starts from a completely clean slate rather than conforming to the specifications of a large free-electron laser (FEL) user facility, to optimize the entire instrumentation towards fundamental measurements of the mechanism of light absorption and excitation energy transfer. A multidisciplinary team formed by laser-, accelerator,- X-ray scientists as well as spectroscopists and biochemists optimizes X-ray pulse parameters, in tandem with sample delivery, crystal size, and advanced X-ray detectors. Ultimately, the new capability, attosecond serial X-ray crystallography and spectroscopy, will be applied to one of the most important problems in structural biology, which is to elucidate the dynamics of light reactions, electron transfer and protein structure in photosynthesis.

Photon-in photon-out hard X-ray spectroscopy at the Linac Coherent Light Source

DOE PAGES

Alonso-Mori, Roberto; Sokaras, Dimosthenis; Zhu, Diling; ...

2015-04-15

X-ray free-electron lasers (FELs) have opened unprecedented possibilities to study the structure and dynamics of matter at an atomic level and ultra-fast timescale. Many of the techniques routinely used at storage ring facilities are being adapted for experiments conducted at FELs. In order to take full advantage of these new sources several challenges have to be overcome. They are related to the very different source characteristics and its resulting impact on sample delivery, X-ray optics, X-ray detection and data acquisition. Here it is described how photon-in photon-out hard X-ray spectroscopy techniques can be applied to study the electronic structure andmore » its dynamics of transition metal systems with ultra-bright and ultra-short FEL X-ray pulses. In particular, some of the experimental details that are different compared with synchrotron-based setups are discussed and illustrated by recent measurements performed at the Linac Coherent Light Source.« less

Sub-cycle control of terahertz high-harmonic generation by dynamical Bloch oscillations

NASA Astrophysics Data System (ADS)

Schubert, O.; Hohenleutner, M.; Langer, F.; Urbanek, B.; Lange, C.; Huttner, U.; Golde, D.; Meier, T.; Kira, M.; Koch, S. W.; Huber, R.

2014-02-01

Ultrafast charge transport in strongly biased semiconductors is at the heart of high-speed electronics, electro-optics and fundamental solid-state physics. Intense light pulses in the terahertz spectral range have opened fascinating vistas. Because terahertz photon energies are far below typical electronic interband resonances, a stable electromagnetic waveform may serve as a precisely adjustable bias. Novel quantum phenomena have been anticipated for terahertz amplitudes, reaching atomic field strengths. We exploit controlled (multi-)terahertz waveforms with peak fields of 72 MV cm-1 to drive coherent interband polarization combined with dynamical Bloch oscillations in semiconducting gallium selenide. These dynamics entail the emission of phase-stable high-harmonic transients, covering the entire terahertz-to-visible spectral domain between 0.1 and 675 THz. Quantum interference of different ionization paths of accelerated charge carriers is controlled via the waveform of the driving field and explained by a quantum theory of inter- and intraband dynamics. Our results pave the way towards all-coherent terahertz-rate electronics.

Ultrafast electron diffraction and electron microscopy: present status and future prospects

NASA Astrophysics Data System (ADS)

Ishchenko, A. A.; Aseyev, S. A.; Bagratashvili, V. N.; Panchenko, V. Ya; Ryabov, E. A.

2014-07-01

Acting as complementary research tools, high time-resolved spectroscopy and diffractometry techniques proceeding from various physical principles open up new possibilities for studying matter with necessary integration of the 'structure-dynamics-function' triad in physics, chemistry, biology and materials science. Since the 1980s, a new field of research has started at the leading research laboratories, aimed at developing means of filming the coherent dynamics of nuclei in molecules and fast processes in biological objects ('atomic and molecular movies'). The utilization of ultrashort laser pulse sources has significantly modified traditional electron beam approaches to and provided high space-time resolution for the study of materials. Diffraction methods using frame-by-frame filming and the development of the main principles of the study of coherent dynamics of atoms have paved the way to observing wave packet dynamics, the intermediate states of reaction centers, and the dynamics of electrons in molecules, thus allowing a transition from the kinetics to the dynamics of the phase trajectories of molecules in the investigation of chemical reactions.

Coherent Control of Nanoscale Ballistic Currents in Transition Metal Dichalcogenide ReS2.

PubMed

Cui, Qiannan; Zhao, Hui

2015-04-28

Transition metal dichalcogenides are predicted to outperform traditional semiconductors in ballistic devices with nanoscale channel lengths. So far, experimental studies on charge transport in transition metal dichalcogenides are limited to the diffusive regime. Here we show, using ReS2 as an example, all-optical injection, detection, and coherent control of ballistic currents. By utilizing quantum interference between one-photon and two-photon interband transition pathways, ballistic currents are injected in ReS2 thin film samples by a pair of femtosecond laser pulses. We find that the current decays on an ultrafast time scale, resulting in an electron transport of only a fraction of one nanometer. Following the relaxation of the initially injected momentum, backward motion of the electrons for about 1 ps is observed, driven by the Coulomb force from the oppositely moved holes. We also show that the injected current can be controlled by the phase of the laser pulses. These results demonstrate a new platform to study ballistic transport of nonequilibrium carriers in transition metal dichalcogenides.

Imaging single cells in a beam of live cyanobacteria with an X-ray laser.

PubMed

van der Schot, Gijs; Svenda, Martin; Maia, Filipe R N C; Hantke, Max; DePonte, Daniel P; Seibert, M Marvin; Aquila, Andrew; Schulz, Joachim; Kirian, Richard; Liang, Mengning; Stellato, Francesco; Iwan, Bianca; Andreasson, Jakob; Timneanu, Nicusor; Westphal, Daniel; Almeida, F Nunes; Odic, Dusko; Hasse, Dirk; Carlsson, Gunilla H; Larsson, Daniel S D; Barty, Anton; Martin, Andrew V; Schorb, Sebastian; Bostedt, Christoph; Bozek, John D; Rolles, Daniel; Rudenko, Artem; Epp, Sascha; Foucar, Lutz; Rudek, Benedikt; Hartmann, Robert; Kimmel, Nils; Holl, Peter; Englert, Lars; Duane Loh, Ne-Te; Chapman, Henry N; Andersson, Inger; Hajdu, Janos; Ekeberg, Tomas

2015-02-11

There exists a conspicuous gap of knowledge about the organization of life at mesoscopic levels. Ultra-fast coherent diffractive imaging with X-ray free-electron lasers can probe structures at the relevant length scales and may reach sub-nanometer resolution on micron-sized living cells. Here we show that we can introduce a beam of aerosolised cyanobacteria into the focus of the Linac Coherent Light Source and record diffraction patterns from individual living cells at very low noise levels and at high hit ratios. We obtain two-dimensional projection images directly from the diffraction patterns, and present the results as synthetic X-ray Nomarski images calculated from the complex-valued reconstructions. We further demonstrate that it is possible to record diffraction data to nanometer resolution on live cells with X-ray lasers. Extension to sub-nanometer resolution is within reach, although improvements in pulse parameters and X-ray area detectors will be necessary to unlock this potential.

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching

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

Lemke, Henrik T.; Kjær, Kasper S.; Hartsock, Robert

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born–Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersionmore » of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.« less

Macrospin dynamics in antiferromagnets triggered by sub-20 femtosecond injection of nanomagnons.

PubMed

Bossini, D; Dal Conte, S; Hashimoto, Y; Secchi, A; Pisarev, R V; Rasing, Th; Cerullo, G; Kimel, A V

2016-02-05

The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridging the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter in the Heisenberg antiferromagnet KNiF3 triggered by the impulsive optical generation of spin excitations with the shortest possible nanometre wavelength and femtosecond period. Our magneto-optical pump-probe experiments also demonstrate the coherent manipulation of the phase and amplitude of these femtosecond nanomagnons, whose frequencies are defined by the exchange energy. These findings open up opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and strongly correlated materials; they also suggest that nanospintronics and nanomagnonics can employ coherently controllable spin waves with frequencies in the 20 THz domain.

Macrospin dynamics in antiferromagnets triggered by sub-20 femtosecond injection of nanomagnons

NASA Astrophysics Data System (ADS)

Bossini, D.; Dal Conte, S.; Hashimoto, Y.; Secchi, A.; Pisarev, R. V.; Rasing, Th.; Cerullo, G.; Kimel, A. V.

2016-02-01

The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridging the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter in the Heisenberg antiferromagnet KNiF3 triggered by the impulsive optical generation of spin excitations with the shortest possible nanometre wavelength and femtosecond period. Our magneto-optical pump-probe experiments also demonstrate the coherent manipulation of the phase and amplitude of these femtosecond nanomagnons, whose frequencies are defined by the exchange energy. These findings open up opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and strongly correlated materials; they also suggest that nanospintronics and nanomagnonics can employ coherently controllable spin waves with frequencies in the 20 THz domain.

Spectral domain optical coherence tomography of multi-MHz A-scan rates at 1310 nm range and real-time 4D-display up to 41 volumes/second

PubMed Central

Choi, Dong-hak; Hiro-Oka, Hideaki; Shimizu, Kimiya; Ohbayashi, Kohji

2012-01-01

An ultrafast frequency domain optical coherence tomography system was developed at A-scan rates between 2.5 and 10 MHz, a B-scan rate of 4 or 8 kHz, and volume-rates between 12 and 41 volumes/second. In the case of the worst duty ratio of 10%, the averaged A-scan rate was 1 MHz. Two optical demultiplexers at a center wavelength of 1310 nm were used for linear-k spectral dispersion and simultaneous differential signal detection at 320 wavelengths. The depth-range, sensitivity, sensitivity roll-off by 6 dB, and axial resolution were 4 mm, 97 dB, 6 mm, and 23 μm, respectively. Using FPGAs for FFT and a GPU for volume rendering, a real-time 4D display was demonstrated at a rate up to 41 volumes/second for an image size of 256 (axial) × 128 × 128 (lateral) voxels. PMID:23243560

Field transients of coherent terahertz synchrotron radiation accessed via time-resolving and correlation techniques

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

Pohl, A.; Hübers, H.-W.; Institute of Optical Sensor Systems, German Aerospace Center

2016-03-21

Decaying oscillations of the electric field in repetitive pulses of coherent synchrotron radiation in the terahertz frequency range was evaluated by means of time-resolving and correlation techniques. Comparative analysis of real-time voltage transients of the electrical response and interferograms, which were obtained with an ultrafast zero-bias Schottky diode detector and a Martin-Puplett interferometer, delivers close values of the pulse duration. Consistent results were obtained via the correlation technique with a pair of Golay Cell detectors and a pair of resonant polarisation-sensitive superconducting detectors integrated on one chip. The duration of terahertz synchrotron pulses does not closely correlate with the durationmore » of single-cycle electric field expected for the varying size of electron bunches. We largely attribute the difference to the charge density oscillations in electron bunches and to the low-frequency spectral cut-off imposed by both the synchrotron beamline and the coupling optics of our detectors.« less

Direct observation of ultrafast coherent exciton dynamics in helical π-stacks of self-assembled perylene bisimides

PubMed Central

Sung, Jooyoung; Kim, Pyosang; Fimmel, Benjamin; Würthner, Frank; Kim, Dongho

2015-01-01

Ever since the discovery of dye self-assemblies in nature, there have been tremendous efforts to exploit biomimetic supramolecular assemblies for tailored artificial photon processing materials. This feature necessarily has resulted in an increasing demand for understanding exciton dynamics in the dye self-assemblies. In a sharp contrast with J-type aggregates, however, the detailed observation of exciton dynamics in H-type aggregates has remained challenging. In this study, as we succeed in measuring transient fluorescence from Frenkel state of π-stacked perylene tetracarboxylic acid bisimide dimer and oligomer aggregates, we present an experimental demonstration on Frenkel exciton dynamics of archetypal columnar π–π stacks of dyes. The analysis of the vibronic peak ratio of the transient fluorescence spectra reveals that unlike the simple π-stacked dimer, the photoexcitation energy in the columnar π-stacked oligomer aggregates is initially delocalized over at least three molecular units and moves coherently along the chain in tens of femtoseconds, preceding excimer formation process. PMID:26492820

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching

DOE PAGES

Lemke, Henrik T.; Kjær, Kasper S.; Hartsock, Robert; ...

2017-05-24

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born–Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersionmore » of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.« less

On The Geometric Nature of ``Singlet Fission'' in Certain Crystalline Conjugated Polymers

NASA Astrophysics Data System (ADS)

Rahman, Noah

2013-03-01

In recent years, the coherent fission of low-lying singlet electronic excitations in conjugated polymers has attracted interest as a possible way to exceed the Shockley-Queisser limit in organic photovoltaics. Femtosecond spectroscopic and fluorescence measurements of such singlets and the resulting triplets in crystalline anthracene, tetracene and naphthalene reveal curious phenomena associated with certain vibrational modes, such as ultrafast propagation on a timescale inconsistent with conventional intersystem crossing, long-lived electronic coherence, and triplet magnetic anisotropy whose structure is consistent across all three materials. This conflicts with NRG and quantum chemical simulations, which posit isotropic triplets. I explain this by a dynamical Rashba spin-orbit interaction that decays as R-6. This arises from a geometric SU(2) gauge potential generated by a nuclear-motion-induced parametric near-degeneracy of the molecular electronic states. The anisotropy is shown to follow from the work of Affleck and Oshikawa on spin one-half Heisenberg chains. Possible directions for future work are discussed, especially with regard to adiabatic pumping and topological insulators.

Ultrafast spectroscopy of coherent phonon in carbon nanotubes using sub-5-fs visible pulses

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

Kobayashi, Takayoshi; JST, CREST, 5 Sanbancho, Chiyoda-ku, Tokyo 102-0075 Japan; Department of Electrophysics, National Chiao Tung University, Hsinchu 30010, Taiwan

2016-02-01

In the last two decades, nano materials are attracting many scientists’ interest for both basic and application viewpoints. In order to understand the properties of nano systems it is needed to understand the dynamic properties which control the specific properties of the systems. All the primary processes in nano systems are taking place in femtosecond regime. Our group has been able to stably generate visible to near-infrared sub-5-fs laser pulses using a noncollinear optical parametric amplifier (NOPA) by the combination of various novel techniques including non-collinear optical parametric amplifier, pulse compression by a prism pair and grating pair. We applymore » the sub-5-fs pulses to study real-time coherent phonon in a one-dimensional system of carbon nanotubes. We determine exciton-phonon coupling mechanisms by observing the breathing mode in semiconducting carbon nanotubes and show the effect of electronic transition affected by the vibrational mode.« less

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching

NASA Astrophysics Data System (ADS)

Lemke, Henrik T.; Kjær, Kasper S.; Hartsock, Robert; van Driel, Tim B.; Chollet, Matthieu; Glownia, James M.; Song, Sanghoon; Zhu, Diling; Pace, Elisabetta; Matar, Samir F.; Nielsen, Martin M.; Benfatto, Maurizio; Gaffney, Kelly J.; Collet, Eric; Cammarata, Marco

2017-05-01

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born-Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersion of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.

Relation between magnetization and Faraday angles produced by ultrafast spin-flip processes within the three-level Λ-type system

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

Hinschberger, Y.; Lavoine, J. P.

2015-08-07

Ultrafast magneto-optical (MO) experiments constitute a powerful tool to explore the magnetization dynamics of diverse materials. Over the last decade, there have been many theoretical and experimental developments on this subject. However, the relation between the magnetization dynamics and the transient MO response still remains unclear. In this work, we calculate the magnetization of a material, as well as the magneto-optical rotation and ellipticity angles measured in a single-beam experiment. Then, we compare the magnetization to the MO response. The magnetic material is modeled by a three-level Λ-type system, which represents a simple model to describe MO effects induced bymore » an ultrafast laser pulse. Our calculations use the density matrix formalism, while the dynamics of the system is obtained by solving the Lindblad equation taking into account population relaxation and dephasing processes. Furthermore, we consider the Faraday rotation of the optical waves that simultaneously causes spin-flip. We show that the Faraday angles remain proportional to the magnetization only if the system has reached the equilibrium-state, and that this proportionality is directly related to the population and coherence decay rates. For the non-equilibrium situation, the previous proportionality relation is no longer valid. We show that our model is able to interpret some recent experimental results obtained in a single-pulse experiment. We further show that, after a critical pulse duration, the decrease of the ellipticity as a function of the absorbed energy is a characteristic of the system.« less

Role of many-body effects in the coherent dynamics of excitons in low-temperature-grown GaAs

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

Webber, D.; Hacquebard, L.; Hall, K. C.

2015-10-05

Femtosecond four-wave mixing experiments on low-temperature-grown (LT-) GaAs indicate a polarization-dependent nonlinear optical response at the exciton, which we attribute to Coulomb-mediated coupling between excitons and electron-hole pairs simultaneously excited by the broad-bandwidth laser pulses. Strong suppression of the exciton response through screening by carriers injected by a third pump pulse was observed, an effect that is transient due to rapid carrier trapping. Our findings highlight the need to account for the complex interplay of disorder and many-body effects in the design of ultrafast optoelectronic devices using this material.

Laser applications and system considerations in ocular imaging

PubMed Central

Elsner, Ann E.; Muller, Matthew S.

2009-01-01

We review laser applications for primarily in vivo ocular imaging techniques, describing their constraints based on biological tissue properties, safety, and the performance of the imaging system. We discuss the need for cost effective sources with practical wavelength tuning capabilities for spectral studies. Techniques to probe the pathological changes of layers beneath the highly scattering retina and diagnose the onset of various eye diseases are described. The recent development of several optical coherence tomography based systems for functional ocular imaging is reviewed, as well as linear and nonlinear ocular imaging techniques performed with ultrafast lasers, emphasizing recent source developments and methods to enhance imaging contrast. PMID:21052482

Generation of Gigawatt Circularly Polarized Attosecond-Pulse Pairs

NASA Astrophysics Data System (ADS)

Hu, K.; Wu, H.-C.

2017-12-01

A novel scheme for generating a pair of gigawatt attosecond pulses by coherent Thomson scattering from relativistic electron sheets is proposed. With a circularly polarized relativistic laser pulse, the scattered x-ray signal can have a saddlelike temporal profile, where the lower electromagnetic frequencies are found mostly in the center region of this saddlelike profile. By filtering out the latter, we can obtain two few-attosecond pulses separated by a subfemtosecond interval, which is tunable by controlling the energy of the sheet electrons. Such a pulse pair can be useful for an attosecond pump probe at an unprecedented time resolution and for ultrafast chiral studies in molecules and materials.

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.

Coherent X-ray diffraction from collagenous soft tissues

PubMed Central

Berenguer de la Cuesta, Felisa; Wenger, Marco P. E.; Bean, Richard J.; Bozec, Laurent; Horton, Michael A.; Robinson, Ian K.

2009-01-01

Coherent X-ray diffraction has been applied in the imaging of inorganic materials with great success. However, its application to biological specimens has been limited to some notable exceptions, due to the induced radiation damage and the extended nature of biological samples, the last limiting the application of most part of the phasing algorithms. X-ray ptychography, still under development, is a good candidate to overcome such difficulties and become a powerful imaging method for biology. We describe herein the feasibility of applying ptychography to the imaging of biological specimens, in particular collagen rich samples. We report here speckles in diffraction patterns from soft animal tissue, obtained with an optimized small angle X-ray setup that exploits the natural coherence of the beam. By phasing these patterns, dark field images of collagen within tendon, skin, bone, or cornea will eventually be obtained with a resolution of 60–70 nm. We present simulations of the contrast mechanism in collagen based on atomic force microscope images of the samples. Simulations confirmed the ‘speckled’ nature of the obtained diffraction patterns. Once inverted, the patterns will show the disposition and orientation of the fibers within the tissue, by enhancing the phase contrast between protein and no protein regions of the sample. Our work affords the application of the most innovative coherent X-ray diffraction tools to the study of biological specimens, and this approach will have a significant impact in biology and medicine because it overcomes many of the limits of current microscopy techniques. PMID:19706395

Coherent X-ray diffraction from collagenous soft tissues.

PubMed

Berenguer de la Cuesta, Felisa; Wenger, Marco P E; Bean, Richard J; Bozec, Laurent; Horton, Michael A; Robinson, Ian K

2009-09-08

Coherent X-ray diffraction has been applied in the imaging of inorganic materials with great success. However, its application to biological specimens has been limited to some notable exceptions, due to the induced radiation damage and the extended nature of biological samples, the last limiting the application of most part of the phasing algorithms. X-ray ptychography, still under development, is a good candidate to overcome such difficulties and become a powerful imaging method for biology. We describe herein the feasibility of applying ptychography to the imaging of biological specimens, in particular collagen rich samples. We report here speckles in diffraction patterns from soft animal tissue, obtained with an optimized small angle X-ray setup that exploits the natural coherence of the beam. By phasing these patterns, dark field images of collagen within tendon, skin, bone, or cornea will eventually be obtained with a resolution of 60-70 nm. We present simulations of the contrast mechanism in collagen based on atomic force microscope images of the samples. Simulations confirmed the 'speckled' nature of the obtained diffraction patterns. Once inverted, the patterns will show the disposition and orientation of the fibers within the tissue, by enhancing the phase contrast between protein and no protein regions of the sample. Our work affords the application of the most innovative coherent X-ray diffraction tools to the study of biological specimens, and this approach will have a significant impact in biology and medicine because it overcomes many of the limits of current microscopy techniques.

Extending of flat normal dispersion profile in all-solid soft glass nonlinear photonic crystal fibres

NASA Astrophysics Data System (ADS)

Siwicki, Bartłomiej; Kasztelanic, Rafał; Klimczak, Mariusz; Cimek, Jarosław; Pysz, Dariusz; Stępień, Ryszard; Buczyński, Ryszard

2016-06-01

The bandwidth of coherent supercontinuum generated in optical fibres is strongly determined by the all-normal dispersion characteristic of the fibre. We investigate all-normal dispersion limitations in all-solid oxide-based soft glass photonic crystal fibres with various relative inclusion sizes and lattice constants. The influence of material dispersion on fibre dispersion characteristics for a selected pair of glasses is also examined. A relation between the material dispersion of the glasses and the fibre dispersion has been described. We determined the parameters which limit the maximum range of flattened all-normal dispersion profile achievable for the considered pair of heavy-metal-oxide soft glasses.

Hot and dense plasma probing by soft X-ray lasers

NASA Astrophysics Data System (ADS)

Krůs, M.; Kozlová, M.; Nejdl, J.; Rus, B.

2018-01-01

Soft X-ray lasers, due to their short wavelength, its brightness, and good spatial coherence, are excellent sources for the diagnostics of dense plasmas (up to 1025 cm-3) which are relevant to e.g. inertial fusion. Several techniques and experimental results, which are obtained at the quasi-steady state scheme being collisionally pumped 21.2 nm neon-like zinc laser installed at PALS Research Center, are presented here; among them the plasma density measurement by a double Lloyd mirror interferometer, deflectometer based on Talbot effect measuring plasma density gradients itself, with a following ray tracing postprocessing. Moreover, the high spatial resolution (nm scale) plasma images can be obtained when soft X-ray lasers are used.

GPU-based real-time soft tissue deformation with cutting and haptic feedback.

PubMed

Courtecuisse, Hadrien; Jung, Hoeryong; Allard, Jérémie; Duriez, Christian; Lee, Doo Yong; Cotin, Stéphane

2010-12-01

This article describes a series of contributions in the field of real-time simulation of soft tissue biomechanics. These contributions address various requirements for interactive simulation of complex surgical procedures. In particular, this article presents results in the areas of soft tissue deformation, contact modelling, simulation of cutting, and haptic rendering, which are all relevant to a variety of medical interventions. The contributions described in this article share a common underlying model of deformation and rely on GPU implementations to significantly improve computation times. This consistency in the modelling technique and computational approach ensures coherent results as well as efficient, robust and flexible solutions. Copyright © 2010 Elsevier Ltd. All rights reserved.

Nonlinear phase noise tolerance for coherent optical systems using soft-decision-aided ML carrier phase estimation enhanced with constellation partitioning

NASA Astrophysics Data System (ADS)

Li, Yan; Wu, Mingwei; Du, Xinwei; Xu, Zhuoran; Gurusamy, Mohan; Yu, Changyuan; Kam, Pooi-Yuen

2018-02-01

A novel soft-decision-aided maximum likelihood (SDA-ML) carrier phase estimation method and its simplified version, the decision-aided and soft-decision-aided maximum likelihood (DA-SDA-ML) methods are tested in a nonlinear phase noise-dominant channel. The numerical performance results show that both the SDA-ML and DA-SDA-ML methods outperform the conventional DA-ML in systems with constant-amplitude modulation formats. In addition, modified algorithms based on constellation partitioning are proposed. With partitioning, the modified SDA-ML and DA-SDA-ML are shown to be useful for compensating the nonlinear phase noise in multi-level modulation systems.

Ultrafast visualization of the structural evolution of dense hydrogen towards warm dense matter

NASA Astrophysics Data System (ADS)

Fletcher, Luke

2016-10-01

Hot dense hydrogen far from equilibrium is ubiquitous in nature occurring during some of the most violent and least understood events in our universe such as during star formation, supernova explosions, and the creation of cosmic rays. It is also a state of matter important for applications in inertial confinement fusion research and in laser particle acceleration. Rapid progress occurred in recent years characterizing the high-pressure structural properties of dense hydrogen under static or dynamic compression. Here, we show that spectrally and angularly resolved x-ray scattering measure the thermodynamic properties of dense hydrogen and resolve the ultrafast evolution and relaxation towards thermodynamic equilibrium. These studies apply ultra-bright x-ray pulses from the Linac Coherent Light (LCLS) source. The interaction of rapidly heated cryogenic hydrogen with a high-peak power optical laser is visualized with intense LCLS x-ray pulses in a high-repetition rate pump-probe setting. We demonstrate that electron-ion coupling is affected by the small number of particles in the Debye screening cloud resulting in much slower ion temperature equilibration than predicted by standard theory. This work was supported by the DOE Office of Science, Fusion Energy Science under FWP 100182.

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

Zhang, Bing-Bing; Liu, Jian; Wei, Xu

We investigate the transient photoexcited lattice dynamics in a layered perovskite Mott insulator Sr2IrO4 film by femtosecond X-ray diffraction using a laser plasma-based X-ray source. The ultrafast structural dynamics of Sr2IrO4 thin films are determined by observing the shift and broadening of (0012) Bragg diffraction after excitation by 1.5 eV and 3.0 eV pump photons for films with different thicknesses. The observed transient lattice response can be well interpreted as a distinct three-step dynamics due to the propagation of coherent acoustic phonons generated by photoinduced quasiparticles (QPs). Employing a normalized phonon propagation model, we found that the photoinduced angular shiftsmore » of the Bragg peak collapse into a universal curve after introducing normalizedn coordinates to account for different thicknesses and pump photon energies, pinpointing the origin of the lattice distortion and its early evolution. In addition, a transient photocurrent measurement indicates that the photoinduced QPs are charge neutral excitons. Mapping the phonon propagation and correlating its dynamics with the QP by ultrafast X-ray diffraction (UXRD) establish a powerful way to study electron-phonon coupling and uncover the exotic physics in strongly correlated systems under nonequilibrium conditions.« less

Imaging nanoscale spatial modulation of a relativistic electron beam with a MeV ultrafast electron microscope

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

Lu, Chao; Jiang, Tao; Liu, Shengguang

Here, an accelerator-based MeV ultrafast electron microscope (MUEM) has been proposed as a promising tool to the study structural dynamics at the nanometer spatial scale and the picosecond temporal scale. Here, we report experimental tests of a prototype MUEM where high quality images with nanoscale fine structures were recorded with a pulsed ~3 MeV picosecond electron beam. The temporal and spatial resolutions of the MUEM operating in the single-shot mode are about 4 ps (FWHM) and 100 nm (FWHM), corresponding to a temporal-spatial resolution of 4 × 10 –19 sm, about 2 orders of magnitude higher than that achieved withmore » state-of-the-art single-shot keV UEM. Using this instrument, we offer the demonstration of visualizing the nanoscale periodic spatial modulation of an electron beam, which may be converted into longitudinal density modulation through emittance exchange to enable production of high-power coherent radiation at short wavelengths. Our results mark a great step towards single-shot nanometer-resolution MUEMs and compact intense x-ray sources that may have widespread applications in many areas of science.« less

Imaging nanoscale spatial modulation of a relativistic electron beam with a MeV ultrafast electron microscope

DOE PAGES

Lu, Chao; Jiang, Tao; Liu, Shengguang; ...

2018-03-12

Here, an accelerator-based MeV ultrafast electron microscope (MUEM) has been proposed as a promising tool to the study structural dynamics at the nanometer spatial scale and the picosecond temporal scale. Here, we report experimental tests of a prototype MUEM where high quality images with nanoscale fine structures were recorded with a pulsed ~3 MeV picosecond electron beam. The temporal and spatial resolutions of the MUEM operating in the single-shot mode are about 4 ps (FWHM) and 100 nm (FWHM), corresponding to a temporal-spatial resolution of 4 × 10 –19 sm, about 2 orders of magnitude higher than that achieved withmore » state-of-the-art single-shot keV UEM. Using this instrument, we offer the demonstration of visualizing the nanoscale periodic spatial modulation of an electron beam, which may be converted into longitudinal density modulation through emittance exchange to enable production of high-power coherent radiation at short wavelengths. Our results mark a great step towards single-shot nanometer-resolution MUEMs and compact intense x-ray sources that may have widespread applications in many areas of science.« less

Modeling of Optoelectronic Devices

NASA Technical Reports Server (NTRS)

Li, Jian-Zhong; Woo, Alex C. (Technical Monitor)

2000-01-01

Ultrafast modulation of semiconductor quantum well (QW) laser is of technological importance for information technology. Improvement by order(s) of magnitude in data transfer rate is possible as terahertz (THz) radiation is available for heating the laser at picosecond time scale. Optical gain modulation in the QW is achieved via temperature modulation of electron-hole plasma (EHP). Applications include free-space THz communication, optical switching, and pulse generation. The EHP in the semiconductor QW is described with a two-band model. Semiconductor Bloch equations with many-body effects are used to derive a hydrodynamical model for the active QW region. Because of ultrafast carrier-carrier scatterings in the order of 50 fs, EHP follows quasiequilibrium Fermi-Dirac distributions and THz field interacts incoherently with it. Carrier-longitudinal optical (LO) phonon scatterings and coherent laser-EHP interaction are treated microscopically in our physical model. A set of hydrodynamical equations for plasma density, temperature, and laser envelop amplitude are derived and Runge-Kutta method is adopted for numerical simulation. A typical 8 nm GaAs/Al(0.3)Ga(0.7) As single QW at 300 K is used. Additional information is contained in the original extended abstract.

Soft x-ray speckle from rough surfaces

NASA Astrophysics Data System (ADS)

Porter, Matthew Stanton

Dynamic light scattering has been of great use in determining diffusion times for polymer solutions. At the same time, polymer thin films are becoming of increasing importance, especially in the semiconductor industry where they are used as photoresists and interlevel dielectrics. As the dimensions of these devices decrease we will reach a point where lasers will no longer be able to probe the length scales of interest. Current laser wavelengths limit the size of observable diffusion lengths to 180-700 nm. This dissertation will discuss attempts at pushing dynamic fight scattering experiments into the soft x-ray region so that we can examine fluctuations in polymer thin films on the molecular length scale. The dissertation explores the possibility of carrying out a dynamic light scattering experiment in the soft x-ray regime. A detailed account of how to meet the basic requirements for a coherent scattering experiment in the soft x-ray regime win be given. In addition, a complete description of the chamber design will be discussed. We used our custom designed scattering chamber to collect reproducible coherent soft x-ray scattering data from etched silicon wafers and from polystyrene coated silicon wafers. The data from the silicon wafers followed the statistics for a well-developed speckle pattern while the data from the polystyrene films exhibited Poisson statistics. We used the data from both the etched wafers and the polystyrene coated wafers to place a lower limit of ~20 Å on the RMS surface roughness of samples which will produce well defined speckle patterns for the current detector setup. Future experiments which use the criteria set forth in this dissertation have the opportunity to be even more successful than this dissertation project.

Comparative Assessment of Conventional Papanicolaou and Modified Ultrafast Papanicolaou Stains in Fine Needle Aspiration Samples and Body Fluids.

PubMed

Arul, P; Eniya, S; Pushparaj, Magesh; Masilamani, Suresh; Kanmani, P; Lingasamy, C

2018-01-01

Conventional Papanicolaou (Pap) stain has undergone many modifications; of these, ultrafast Pap stain is the most popular as it shortens the turnaround time of reporting. Application of modified ultrafast Pap (MUFP) stain in the evaluation of fine needle aspiration (FNA) samples and body fluids are scanty. To evaluate the utility of MUFP stain in various FNA samples and body fluids and compare the findings with those of conventional Pap stain. In this cross-sectional study, two wet-fixed and two airdried smears from each sample [301 samples (255 FNA samples and 46 body fluids)] were prepared and stained by the conventional Pap and MUFP stains, respectively. Concordant and discordant rate was calculated. Quality index (QI) of MUFP stain was assessed by background, overall staining, cell morphology, and nuclear characteristics. MUFP-stained smears were also categorized into excellent, good, and fair. The concordance rate for MUFP stain was 100%. QI of MUFP stain for breast, thyroid, lymph node, soft tissue, salivary gland, and body fluids was 0.9, 0.93, 0.95, 1, 0.94, and 1, respectively. Excellent quality of stain was noted in 53.2% and good in 24.6% of the cases allowing easy diagnosis. In 22.2% of fair cases, diagnosis was possible with some difficulties. Our study concluded that MUFP stain could be considered as a rapid and reliable diagnostic tool and can be applied on a regular basis in FNA samples and body fluids to offer immediate diagnosis. However, caution should be taken while reporting certain MUFP-stained smears to avoid over/under diagnosis.

Isolated elliptically polarized attosecond soft X-ray with high-brilliance using polarization gating of harmonics from relativistic plasmas at oblique incidence.

PubMed

Chen, Zi-Yu; Li, Xiao-Ya; Li, Bo-Yuan; Chen, Min; Liu, Feng

2018-02-19

The production of intense isolated attosecond pulse is a major goal in ultrafast research. Recent advances in high harmonic generation from relativistic plasma mirrors under oblique incidence interactions gave rise to photon-rich attosecond pulses with circular or elliptical polarization. However, to achieve an isolated elliptical attosecond pulse via polarization gating using currently available long driving pulses remains a challenge, because polarization gating of high harmonics from relativistic plasmas is assumed only possible at normal or near-normal incidence. Here we numerically demonstrate a scheme around this problem. We show that via control of plasma dynamics by managing laser polarization, it is possible to gate an intense single attosecond pulse with high ellipticity extending to the soft X-ray regime at oblique incidence. This approach thus paves the way towards a powerful tool enabling high-time-resolution probe of dynamics of chiral systems and magnetic materials with current laser technology.

Element-selective investigation of domain structure in CoPd and FePd alloys using small-angle soft X-ray scattering

NASA Astrophysics Data System (ADS)

Weier, C.; Adam, R.; Frömter, R.; Bach, J.; Winkler, G.; Kobs, A.; Oepen, H. P.; Grychtol, P.; Kapteyn, H. C.; Murnane, M. M.; Schneider, C. M.

2014-03-01

Recent optical pump-probe experiments on magnetic multilayers and alloys identified perpendicular spin superdiffusion as one of possible mechanisms responsible for femtosecond magnetization dynamics. On the other hand, no strong evidence for the ultrafast lateral spin transport has been reported, so far. To address this question, we studied magnetic domain structure of CoPd and FePd thin films using small-angle scattering of soft X-rays. By tuning the synchrotron-generated X-rays to the absorption edges of Fe or Co we recorded Fourier images of the magnetic domain structure corresponding to a chosen element. Applying in - situ magnetic fields resulted in pronounced rearrangement of domain structure that was clearly observed in scattering images. Our analysis of both the stand-alone, as well as magnetically coupled CoPd/FePd layers provides insight into the formation of domains under small magnetic field perturbations and pave the way to better understanding of transient changes expected in magneto-dynamic measurements.

Guiding thermomagnetic avalanches with soft magnetic stripes

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

Vlasko-Vlasov, V. K.; Colauto, F.; Benseman, T.

We demonstrate the potential for manipulating the ultrafast dynamics of thermomagnetic flux avalanches (TMA) in superconducting films with soft magnetic stripes deposited on the film. By tuning the in-plane magnetization of the stripes, we induce lines of strong magnetic potentials for Abrikosov vortices, resulting in guided slow motion of vortices along the stripe edges and preferential bursts of TMA along the stripes. Furthermore, we show that transversely polarized stripes can reduce the TMA size by diverting magnetic flux away from the major trunk of the TMA into interstripe gaps. Our data indicate that TMAs are launched from locations with enhancedmore » vortex entry barrier, where flux accumulation followed by accelerated vortex discharge significantly reduces the threshold of the applied field ramping speed required for the creation of TMAs. Finally, vortex-antivortex annihilation at the moving front of an expanding TMA can account for the enhanced TMA activity in the receding branches of the sample's magnetization cycle and the preferred propagation of TMAs into maximum trapped flux regions.« less

Guiding thermomagnetic avalanches with soft magnetic stripes

NASA Astrophysics Data System (ADS)

Vlasko-Vlasov, V. K.; Colauto, F.; Benseman, T.; Rosenmann, D.; Kwok, W.-K.

2017-12-01

We demonstrate the potential for manipulating the ultrafast dynamics of thermomagnetic flux avalanches (TMA) in superconducting films with soft magnetic stripes deposited on the film. By tuning the in-plane magnetization of the stripes, we induce lines of strong magnetic potentials for Abrikosov vortices, resulting in guided slow motion of vortices along the stripe edges and preferential bursts of TMA along the stripes. Furthermore, we show that transversely polarized stripes can reduce the TMA size by diverting magnetic flux away from the major trunk of the TMA into interstripe gaps. Our data indicate that TMAs are launched from locations with enhanced vortex entry barrier, where flux accumulation followed by accelerated vortex discharge significantly reduces the threshold of the applied field ramping speed required for the creation of TMAs. Finally, vortex-antivortex annihilation at the moving front of an expanding TMA can account for the enhanced TMA activity in the receding branches of the sample's magnetization cycle and the preferred propagation of TMAs into maximum trapped flux regions.

Nanometer-scale characterization of laser-driven plasmas, compression, shocks and phase transitions, by coherent small angle x-ray scattering

NASA Astrophysics Data System (ADS)

Kluge, Thomas

2015-11-01

Combining ultra-intense short-pulse and high-energy long-pulse lasers, with brilliant coherent hard X-ray FELs, such as the Helmholtz International Beamline for Extreme Fields (HIBEF) under construction at the HED Instrument of European XFEL, or MEC at LCLS, holds the promise to revolutionize our understanding of many High Energy Density Physics phenomena. Examples include the relativistic electron generation, transport, and bulk plasma response, and ionization dynamics and heating in relativistic laser-matter interactions, or the dynamics of laser-driven shocks, quasi-isentropic compression, and the kinetics of phase transitions at high pressure. A particularly promising new technique is the use of coherent X-ray diffraction to characterize electron density correlations, and by resonant scattering to characterize the distribution of specific charge-state ions, either on the ultrafast time scale of the laser interaction, or associated with hydrodynamic motion. As well one can image slight density changes arising from phase transitions inside of shock-compressed high pressure matter. The feasibility of coherent diffraction techniques in laser-driven matter will be discussed. including recent results from demonstration experiments at MEC. Among other things, very sharp density changes from laser-driven compression are observed, having an effective step width of 10 nm or smaller. This compares to a resolution of several hundred nm achievedpreviously with phase contrast imaging. and on behalf of HIBEF User Consortium, for the Helmholtz International Beamline for Extreme Fields at the European XFEL.

Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales

DOE PAGES

Ulvestad, A.; Cherukara, M. J.; Harder, R.; ...

2017-08-29

Mesoscale thermal transport is of fundamental interest and practical importance in materials such as thermoelectrics. Coherent lattice vibrations (acoustic phonons) govern thermal transport in crystalline solids and are affected by the shape, size, and defect density in nanoscale materials. The advent of hard x-ray free electron lasers (XFELs) capable of producing ultrafast x-ray pulses has significantly impacted the understanding of acoustic phonons by enabling their direct study with x-rays. However, previous studies have reported ensemble-averaged results that cannot distinguish the impact of mesoscale heterogeneity on the phonon dynamics. Here we use Bragg coherent diffractive imaging (BCDI) to resolve the 4Dmore » evolution of the acoustic phonons in a single zinc oxide rod with a spatial resolution of 50 nm and a temporal resolution of 25 picoseconds. We observe homogeneous (lattice breathing/rotation) and inhomogeneous (shear) acoustic phonon modes, which are compared to finite element simulations. We investigate the possibility of changing phonon dynamics by altering the crystal through acid etching. Lastly, we find that the acid heterogeneously dissolves the crystal volume, which will significantly impact the phonon dynamics. In general, our results represent the first step towards understanding the effect of structural properties at the individual crystal level on phonon dynamics.« less

Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales

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

Ulvestad, A.; Cherukara, M. J.; Harder, R.

Mesoscale thermal transport is of fundamental interest and practical importance in materials such as thermoelectrics. Coherent lattice vibrations (acoustic phonons) govern thermal transport in crystalline solids and are affected by the shape, size, and defect density in nanoscale materials. The advent of hard x-ray free electron lasers (XFELs) capable of producing ultrafast x-ray pulses has significantly impacted the understanding of acoustic phonons by enabling their direct study with x-rays. However, previous studies have reported ensemble-averaged results that cannot distinguish the impact of mesoscale heterogeneity on the phonon dynamics. Here we use Bragg coherent diffractive imaging (BCDI) to resolve the 4Dmore » evolution of the acoustic phonons in a single zinc oxide rod with a spatial resolution of 50 nm and a temporal resolution of 25 picoseconds. We observe homogeneous (lattice breathing/rotation) and inhomogeneous (shear) acoustic phonon modes, which are compared to finite element simulations. We investigate the possibility of changing phonon dynamics by altering the crystal through acid etching. Lastly, we find that the acid heterogeneously dissolves the crystal volume, which will significantly impact the phonon dynamics. In general, our results represent the first step towards understanding the effect of structural properties at the individual crystal level on phonon dynamics.« less

Combining coherent hard X-ray tomographies with phase retrieval to generate three-dimensional models of forming bone

NASA Astrophysics Data System (ADS)

Bortel, Emely L.; Langer, Max; Rack, Alexander; Forien, Jean-Baptiste; Duda, Georg N.; Fratzl, Peter; Zaslansky, Paul

2017-11-01

Holotomography, a phase sensitive synchrotron-based μCT modality, is a quantitative 3D imaging method. By exploiting partial spatial X-ray coherence, bones can be imaged volumetrically with high resolution coupled with impressive density sensitivity. This tomographic method reveals the main characteristics of the important tissue compartments in forming bones, including the rapidly-changing soft tissue and the partially or fully mineralized bone regions, while revealing subtle density differences in 3D. Here we show typical results observed within the growing femur bone midshafts of healthy mice that are 1, 3, 7, 10 and 14 days old (postpartum). Our results make use of partially-coherent synchrotron radiation employing inline Fresnel-propagation in multiple tomographic datasets obtained in the imaging beamline ID19 of the ESRF. The exquisite detail creates maps of the juxtaposed soft, partially mineralized and highly mineralized bone revealing the environment in which bone cells create and shape the matrix. This high resolution 3D data is a step towards creating realistic computational models that may be used to study the dynamic processes involved in bone tissue formation and adaptation. Such data will enhance our understanding of the important biomechanical interactions directing maturation and shaping of the bone micro- and macro-geometries.

Longitudinal space charge assisted echo seeding of a free-electron laser with laser-spoiler noise suppression

NASA Astrophysics Data System (ADS)

Hacker, Kirsten

2014-09-01

Seed lasers are employed to improve the temporal coherence of free-electron laser (FEL) light. However, when these seed pulses are short relative to the particle bunch, the noisy, temporally incoherent radiation from the unseeded electrons can overwhelm the coherent, seeded radiation. In this paper, a technique to seed a particle bunch with an external laser is presented in which a new mechanism to improve the contrast between coherent and incoherent free electron laser radiation is employed together with a novel, simplified echo-seeding method. The concept relies on a combination of longitudinal space charge wakes and an echo-seeding technique to make a short, coherent pulse of FEL light together with noise background suppression. Several different simulation codes are used to illustrate the concept with conditions at the soft x-ray free-electron laser in Hamburg, FLASH.

Exchange coupling interaction in L10-FePd/α-Fe nanocomposite magnets with large maximum energy products.

PubMed

Sakuma, Noritsugu; Ohshima, Tsubasa; Shoji, Tetsuya; Suzuki, Yoshihito; Sato, Ryota; Wachi, Ayako; Kato, Akira; Kawai, Yoichiro; Manabe, Akira; Teranishi, Toshiharu

2011-04-26

Nanocomposite magnets (NCMs) consisting of hard and soft magnetic phases are expected to be instrumental in overcoming the current theoretical limit of magnet performance. In this study, structural analyses were performed on L1(0)-FePd/α-Fe NCMs with various hard/soft volume fractions, which were formed by annealing Pd/γ-Fe(2)O(3) heterostructured nanoparticles and pure Pd nanoparticles. The sample with a hard/soft volume ratio of 82/18 formed by annealing at 773 K had the largest maximum energy product (BH(max) = 10.3 MGOe). In such a sample, the interface between the hard and soft phases was coherent and the phase sizes were optimized, both of which effectively induced exchange coupling. This exchange coupling was directly observed by visualizing the magnetic interaction between the hard and soft phases using a first-order reversal curve diagram, which is a valuable tool to improve the magnetic properties of NCMs.

Development of In-situ Resonant Soft X-ray Scattering for Soft Materials at Advanced Light Source

NASA Astrophysics Data System (ADS)

Wang, Cheng; Hexemer, Alexander; Young, Anthony; Padmore, Howard

2014-03-01

Resonant Soft X-ray Scattering was developed at ALS over the past a few years. It combines soft x-ray spectroscopy with x-ray scattering and offers statistical information for 3D chemical morphology over a large sample area. Its unique chemical sensitivity, large accessible size scale, polarization control and high coherence make it a powerful tool for mesoscale chemical/morphological structure characterization for many classes of materials. However, in order to study sciences in naturally occurring conditions, we need to overcome the sample limitations set by the low penetration depth of soft x-rays and requirement of high vacuum. Adapting to the evolving environmental cell designs utilized increasingly in the Electron Microscopy community, we will report our development of customize design liquid/gas environmental cells that will enable soft x-ray scattering experiments on biological, electro-chemical, self-assembly, and hierarchical functional systems in both static and dynamic fashion. Initial RSoXS result of solar fuel membrane assembly/fuel-cell membrane structure in wet cell will be presented.

New Strategic Plan Takes the ALS into the Future

NASA Astrophysics Data System (ADS)

Kirz, J.; Chemla, D. S.; Feinberg, B.; Hussain, Z.; Krebs, G. F.; Padmore, H. A.; Robin, D. S.; Robinson, A. L.; Smith, N. V.; Warwick, T.

2007-01-01

A new strategic plan is in place to upgrade the ALS so it can continue to address fundamental questions, such as size-dependent and dimensional-confinement phenomena at the nanoscale; correlation and complexity in physical, biological, and environmental systems; and temporal evolution, assembly, dynamics and ultrafast phenomena. Moreover, the growing number of ALS users (now exceeding 2,000 per year) requires increased attention. Accordingly, our plan concentrates on projects that will continue to make it possible for ALS users to address grand scientific and technological challenges with incisive world-class tools and quality user support. Our highest priority is to begin top-off operation, in which electrons are injected into the storage ring at intervals of approximately 1 minute. The combination of top-off and concurrent development of small-gap in-vacuum undulators and superconducting undulators will allow an increase in brightness from eight to more than 100 times, depending on the specific undulators and photon energy range. As part of our core mission in the VUV and soft x-ray regions, we plan to exploit these accelerator developments to extend our capabilities for high spatial and temporal resolution and utilize the remarkable coherence properties of the ALS in a new generation of beamlines. Ranked by priority, several proposed beamlines will follow completion of five new beamlines already under construction or funded. The intellectual excitement of the ALS has been a powerful tool in the recruitment and retention of outstanding staff, but additional sustained efforts are required to increase diversity both in gender and in underrepresented groups. To this end, we intend to expand the ALS Doctoral Fellowship Program by giving special emphasis to underrepresented groups. We also envision a distinguished postdoctoral fellowship program with the same emphasis, to increase and diversify our pool of candidates for beamline scientist positions.

Laser speckle visibility acoustic spectroscopy in soft turbid media

NASA Astrophysics Data System (ADS)

Wintzenrieth, Frédéric; Cohen-Addad, Sylvie; Le Merrer, Marie; Höhler, Reinhard

2014-03-01

We image the evolution in space and time of an acoustic wave propagating along the surface of turbid soft matter by shining coherent light on the sample. The wave locally modulates the speckle interference pattern of the backscattered light and the speckle visibility[2] is recorded using a camera. We show both experimentally and theoretically how the temporal and spatial correlations in this pattern can be analyzed to obtain the acoustic wavelength and attenuation length. The technique is validated using shear waves propagating in aqueous foam.[3] It may be applied to other kinds of acoustic wave in different forms of turbid soft matter, such as biological tissues, pastes or concentrated emulsions. Now at Université Lyon 1 (ILM).

TOPICAL REVIEW: Human soft tissue analysis using x-ray or gamma-ray techniques

NASA Astrophysics Data System (ADS)

Theodorakou, C.; Farquharson, M. J.

2008-06-01

This topical review is intended to describe the x-ray techniques used for human soft tissue analysis. X-ray techniques have been applied to human soft tissue characterization and interesting results have been presented over the last few decades. The motivation behind such studies is to provide improved patient outcome by using the data obtained to better understand a disease process and improve diagnosis. An overview of theoretical background as well as a complete set of references is presented. For each study, a brief summary of the methodology and results is given. The x-ray techniques include x-ray diffraction, x-ray fluorescence, Compton scattering, Compton to coherent scattering ratio and attenuation measurements. The soft tissues that have been classified using x-rays or gamma rays include brain, breast, colon, fat, kidney, liver, lung, muscle, prostate, skin, thyroid and uterus.

Direct index of refraction measurements at extreme-ultraviolet and soft-x-ray wavelengths.

PubMed

Rosfjord, Kristine; Chang, Chang; Miyakawa, Ryan; Barth, Holly; Attwood, David

2006-03-10

Coherent radiation from undulator beamlines has been used to directly measure the real and imaginary parts of the index of refraction of several materials at both extreme-ultraviolet and soft-x-ray wavelengths. Using the XOR interferometer, we measure the refractive indices of silicon and ruthenium, essential materials for extreme-ultraviolet lithography. Both materials are tested at wavelength (13.4 nm) and across silicon's L2 (99.8 eV) and L3 (99.2 eV) absorption edges. We further extend this direct phase measurement method into the soft-x-ray region, where measurements of chromium and vanadium are performed around their L3 absorption edges at 574.1 and 512.1 eV, respectively. These are the first direct measurements, to our knowledge, of the real part of the index of refraction made in the soft-x-ray region.

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

PubMed Central

Yu, Ping; Repp, Jascha; Huber, Rupert

2017-01-01

Watching a single molecule move on its intrinsic time scale—one of the central goals of modern nanoscience—calls for measurements that combine ultrafast temporal resolution1–8 with atomic spatial resolution9–30. Steady-state experiments achieve the requisite spatial resolution, as illustrated by direct imaging of individual molecular orbitals using scanning tunnelling microscopy9–11 or the acquisition of tip-enhanced Raman and luminescence spectra with sub-molecular resolution27–29. But tracking the dynamics of a single molecule directly in the time domain faces the challenge that single-molecule excitations need to be confined to an ultrashort time window. A first step towards overcoming this challenge has combined scanning tunnelling microscopy with so-called ‘lightwave electronics”1–8, which uses the oscillating carrier wave of tailored light pulses to directly manipulate electronic motion on time scales faster even than that of a single cycle of light. Here we use such 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 and 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 ~100 fs snapshot images of the structure of the orbital involved, and to reveal through pump-probe measurements coherent molecular vibrations at terahertz frequencies directly in the time domain and with sub-angstrom spatial resolution. We anticipate that the combination of lightwave electronics1–8 and atomic resolution of our approach will open the door to controlling electronic motion inside individual molecules at optical clock rates. PMID:27830788

Generation of sub-two-cycle millijoule infrared pulses in an optical parametric chirped-pulse amplifier and their application to soft x-ray absorption spectroscopy with high-flux high harmonics

NASA Astrophysics Data System (ADS)

Ishii, Nobuhisa; Kaneshima, Keisuke; Kanai, Teruto; Watanabe, Shuntaro; Itatani, Jiro

2018-01-01

An optical parametric chirped-pulse amplifier (OPCPA) based on bismuth triborate (BiB3O6, BIBO) crystals has been developed to deliver 1.5 mJ, 10.1 fs optical pulses around 1.6 μm with a repetition rate of 1 kHz and a stable carrier-envelope phase. The seed and pump pulses of the BIBO-based OPCPA are provided from two Ti:sapphire chirped-pulse amplification (CPA) systems. In both CPA systems, transmission gratings are used in the stretchers and compressors that result in a high throughput and robust operation without causing any thermal problem and optical damage. The seed pulses of the OPCPA are generated by intrapulse frequency mixing of a spectrally broadened continuum, temporally stretched to approximately 5 ps then, and amplified to more than 1.5 mJ. The amplified pulses are compressed in a fused silica block down to 10.1 fs. This BIBO-based OPCPA has been applied to high-flux high harmonic generation beyond the carbon K edge at 284 eV. The high-flux soft-x-ray continuum allows measuring the x-ray absorption near-edge structure of the carbon K edge within 2 min, which is shorter than a typical measurement time using synchrotron-based light sources. This laser-based table-top soft-x-ray source is a promising candidate for ultrafast soft x-ray spectroscopy with femtosecond to attosecond time resolution.

Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses

PubMed Central

Boll, Rebecca; Erk, Benjamin; Coffee, Ryan; Trippel, Sebastian; Kierspel, Thomas; Bomme, Cédric; Bozek, John D.; Burkett, Mitchell; Carron, Sebastian; Ferguson, Ken R.; Foucar, Lutz; Küpper, Jochen; Marchenko, Tatiana; Miron, Catalin; Patanen, Minna; Osipov, Timur; Schorb, Sebastian; Simon, Marc; Swiggers, Michelle; Techert, Simone; Ueda, Kiyoshi; Bostedt, Christoph; Rolles, Daniel; Rudenko, Artem

2016-01-01

Ultrafast electron transfer in dissociating iodomethane and fluoromethane molecules was studied at the Linac Coherent Light Source free-electron laser using an ultraviolet-pump, X-ray-probe scheme. The results for both molecules are discussed with respect to the nature of their UV excitation and different chemical properties. Signatures of long-distance intramolecular charge transfer are observed for both species, and a quantitative analysis of its distance dependence in iodomethane is carried out for charge states up to I21+. The reconstructed critical distances for electron transfer are in good agreement with a classical over-the-barrier model and with an earlier experiment employing a near-infrared pump pulse. PMID:27051675

Giant Electric Field Enhancement in Split Ring Resonators Featuring Nanometer-Sized Gaps

NASA Astrophysics Data System (ADS)

Bagiante, S.; Enderli, F.; Fabiańska, J.; Sigg, H.; Feurer, T.

2015-01-01

Today's pulsed THz sources enable us to excite, probe, and coherently control the vibrational or rotational dynamics of organic and inorganic materials on ultrafast time scales. Driven by standard laser sources THz electric field strengths of up to several MVm-1 have been reported and in order to reach even higher electric field strengths the use of dedicated electric field enhancement structures has been proposed. Here, we demonstrate resonant electric field enhancement structures, which concentrate the incident electric field in sub-diffraction size volumes and show an electric field enhancement as high as ~14,000 at 50 GHz. These values have been confirmed through a combination of near-field imaging experiments and electromagnetic simulations.

Ultrafast compression of graphite observed with sub-ps time resolution diffraction on LCLS

NASA Astrophysics Data System (ADS)

Armstrong, Michael; Goncharov, A.; Crowhurst, J.; Zaug, J.; Radousky, H.; Grivickas, P.; Bastea, S.; Goldman, N.; Stavrou, E.; Belof, J.; Gleason, A.; Lee, H. J.; Nagler, R.; Holtgrewe, N.; Walter, P.; Pakaprenka, V.; Nam, I.; Granados, E.; Presher, C.; Koroglu, B.

2017-06-01

We will present ps time resolution pulsed x-ray diffraction measurements of rapidly compressed highly oriented pyrolytic graphite along its basal plane at the Materials under Extreme Conditions (MEC) sector of the Linac Coherent Light Source (LCLS). These experiments explore the possibility of rapid (<100 ps time scale) material transformations occurring under very highly anisotropic compression conditions. Under such conditions, non-equilibrium mechanisms may play a role in the transformation process. We will present experimental results and simulations which explore this possibility. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Security, LLC under Contract DE-AC52-07NA27344.

Carrier-envelope offset frequency stabilization of an ultrafast semiconductor laser

NASA Astrophysics Data System (ADS)

Jornod, Nayara; Gürel, Kutan; Wittwer, Valentin J.; Brochard, Pierre; Hakobyan, Sargis; Schilt, Stéphane; Waldburger, Dominik; Keller, Ursula; Südmeyer, Thomas

2018-02-01

We present the self-referenced stabilization of the carrier-envelope offset (CEO) frequency of a semiconductor disk laser. The laser is a SESAM-modelocked VECSEL emitting at a wavelength of 1034 nm with a repetition frequency of 1.8 GHz. The 270-fs pulses are amplified to 3 W and compressed to 120 fs for the generation of a coherent octavespanning supercontinuum spectrum. A quasi-common-path f-to-2f interferometer enables the detection of the CEO beat with a signal-to-noise ratio of 30 dB sufficient for its frequency stabilization. The CEO frequency is phase-locked to an external reference with a feedback signal applied to the pump current.

Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction

DOE PAGES

Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul

2017-05-26

We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified, representing (in decreasing strength) elastic scattering, contributions of the electronic coherences created by nonadiabatic couplings in the avoided crossing regime, and inelastic scattering. The former probes the charge density and delivers direct information on the evolving molecular geometry. The latter two contributions are weaker and carry spatial information through the transition charge densities (off-diagonal elements of the charge-density operator). Furthermore, simulations are presented for the nonadiabatic harpooning process in the excitedmore » state of sodium fluoride.« less

Coherent Manipulation of Phonons at the Nanoscale

NASA Astrophysics Data System (ADS)

Yu, Shangjie; Ouyang, Min

Phonons play a key role in almost every physical process, including for example dephasing phenomena of electronic quantum states, electric and heat transports. Therefore, understanding and even manipulating phonons represent a pre-requisite for tailoring phonons-mediated physical processes. In this talk, we will first present how to employ ultrafast optical spectroscopy to probe acoustic phonon modes in colloidal metallic nanoparticles. Furthermore, we have developed various phonon manipulation schemes that can be achieved by a train of optical pulses in time domain to allow selective control of phonon modes. Our theoretical modeling and simulation demonstrates an excellent agreement with experimental results, thus providing a future guideline on more complex phononic control at the nanoscale.