Ultrafast all-optical tuning of direct-gap semiconductor metasurfaces

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

Shcherbakov, Maxim R.; Liu, Sheng; Zubyuk, Varvara V.

Optical metasurfaces are regular quasi-planar nanopatterns that can apply diverse spatial and spectral transformations to light waves. But, metasurfaces are no longer adjustable after fabrication, and a critical challenge is to realise a technique of tuning their optical properties that is both fast and efficient. Here, we experimentally realise an ultrafast tunable metasurface consisting of subwavelength gallium arsenide nanoparticles supporting Mie-type resonances in the near infrared. In using transient reflectance spectroscopy, we demonstrate a picosecond-scale absolute reflectance modulation of up to 0.35 at the magnetic dipole resonance of the metasurfaces and a spectral shift of the resonance by 30 nm,more » both achieved at unprecedentedly low pump fluences of less than 400 μJ cm –2. Our findings thereby enable a versatile tool for ultrafast and efficient control of light using light.« less

Broadband nonlinear optical response of monolayer MoSe2 under ultrafast excitation

NASA Astrophysics Data System (ADS)

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

2018-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2001-03-01

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

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

PubMed

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

2017-04-12

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

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

PubMed Central

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

2015-01-01

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

Ultrafast optical excitation of magnetic skyrmions

NASA Astrophysics Data System (ADS)

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

2015-04-01

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

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

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

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

2014-12-15

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

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

NASA Astrophysics Data System (ADS)

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

2015-01-01

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

Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes

DOE PAGES

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

2016-02-15

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

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.

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

DOE PAGES

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

2017-06-01

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

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

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

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

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

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

PubMed

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

2017-06-01

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

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

PubMed Central

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

2017-01-01

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

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

PubMed

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

2017-08-01

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

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

PubMed

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

2012-01-18

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

Linear and ultrafast nonlinear plasmonics of single nano-objects

NASA Astrophysics Data System (ADS)

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

2017-03-01

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

Quantum simulation of ultrafast dynamics using trapped ultracold atoms.

PubMed

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

2018-05-25

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

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

NASA Astrophysics Data System (ADS)

Smolin, Sergey Y.

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

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.

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

NASA Astrophysics Data System (ADS)

van Howe, James William

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

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

PubMed

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

2017-01-20

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

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

PubMed Central

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

2017-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-01-01

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

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

DTIC Science & Technology

2014-10-01

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

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

Spatially and temporally resolved exciton dynamics and transport in single nanostructures and assemblies

NASA Astrophysics Data System (ADS)

Huang, Libai

2015-03-01

The frontier in solar energy conversion now lies in learning how to integrate functional entities across multiple length scales to create optimal devices. To address this new frontier, I will discuss our recent efforts on elucidating multi-scale energy transfer, migration, and dissipation processes with simultaneous femtosecond temporal resolution and nanometer spatial resolution. We have developed ultrafast microscopy that combines ultrafast spectroscopy with optical microscopy to map exciton dynamics and transport with simultaneous ultrafast time resolution and diffraction-limited spatial resolution. We have employed pump-probe transient absorption microscopy to elucidate morphology and structure dependent exciton dynamics and transport in single nanostructures and molecular assemblies. More specifically, (1) We have applied transient absorption microscopy (TAM) to probe environmental and structure dependent exciton relaxation pathways in sing-walled carbon nanotubes (SWNTs) by mapping dynamics in individual pristine SWNTs with known structures. (2) We have systematically measured and modeled the optical properties of the Frenkel excitons in self-assembled porphyrin tubular aggregates that represent an analog to natural photosynthetic antennae. Using a combination of ultrafast optical microscopy and stochastic exciton modeling, we address exciton transport and relaxation pathways, especially those related to disorder.

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.

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

NASA Astrophysics Data System (ADS)

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

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

Ultrafast Time-Resolved Hard X-Ray Emission Spectroscopy on a Tabletop

NASA Astrophysics Data System (ADS)

Miaja-Avila, Luis; O'Neil, Galen C.; Joe, Young I.; Alpert, Bradley K.; Damrauer, Niels H.; Doriese, William B.; Fatur, Steven M.; Fowler, Joseph W.; Hilton, Gene C.; Jimenez, Ralph; Reintsema, Carl D.; Schmidt, Daniel R.; Silverman, Kevin L.; Swetz, Daniel S.; Tatsuno, Hideyuki; Ullom, Joel N.

2016-07-01

Experimental tools capable of monitoring both atomic and electronic structure on ultrafast (femtosecond to picosecond) time scales are needed for investigating photophysical processes fundamental to light harvesting, photocatalysis, energy and data storage, and optical display technologies. Time-resolved hard x-ray (>3 keV ) spectroscopies have proven valuable for these measurements due to their elemental specificity and sensitivity to geometric and electronic structures. Here, we present the first tabletop apparatus capable of performing time-resolved x-ray emission spectroscopy. The time resolution of the apparatus is better than 6 ps. By combining a compact laser-driven plasma source with a highly efficient array of microcalorimeter x-ray detectors, we are able to observe photoinduced spin changes in an archetypal polypyridyl iron complex [Fe (2 ,2'-bipyridine)3]2 + and accurately measure the lifetime of the quintet spin state. Our results demonstrate that ultrafast hard x-ray emission spectroscopy is no longer confined to large facilities and now can be performed in conventional laboratories with 10 times better time resolution than at synchrotrons. Our results are enabled, in part, by a 100- to 1000-fold increase in x-ray collection efficiency compared to current techniques.

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

NASA Astrophysics Data System (ADS)

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

2014-09-01

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

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

PubMed

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

2015-01-02

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

Femtosecond laser spectroscopy of the rhodopsin photochromic reaction: a concept for ultrafast optical molecular switch creation (ultrafast reversible photoreaction of rhodopsin).

PubMed

Smitienko, Olga; Nadtochenko, Victor; Feldman, Tatiana; Balatskaya, Maria; Shelaev, Ivan; Gostev, Fedor; Sarkisov, Oleg; Ostrovsky, Mikhail

2014-11-11

Ultrafast reverse photoreaction of visual pigment rhodopsin in the femtosecond time range at room temperature is demonstrated. Femtosecond two-pump probe experiments with a time resolution of 25 fs have been performed. The first рump pulse at 500 nm initiated cis-trans photoisomerization of rhodopsin chromophore, 11-cis retinal, which resulted in the formation of the primary ground-state photoproduct within a mere 200 fs. The second pump pulse at 620 nm with a varying delay of 200 to 3750 fs relative to the first рump pulse, initiated the reverse phototransition of the primary photoproduct to rhodopsin. The results of this photoconversion have been observed on the differential spectra obtained after the action of two pump pulses at a time delay of 100 ps. It was found that optical density decreased at 560 nm in the spectral region of bathorhodopsin absorption and increased at 480 nm, where rhodopsin absorbs. Rhodopsin photoswitching efficiency shows oscillations as a function of the time delay between two рump pulses. The quantum yield of reverse photoreaction initiated by the second pump pulse falls within the range 15%±1%. The molecular mechanism of the ultrafast reversible photoreaction of visual pigment rhodopsin may be used as a concept for the development of an ultrafast optical molecular switch.

Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

DOE PAGES

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

2017-07-01

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

Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

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

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

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

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.

WS2 mode-locked ultrafast fiber laser

PubMed Central

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

2015-01-01

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

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

Ultrafast terahertz electrodynamics of photonic and electronic nanostructures

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

Luo, Liang

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

Ultrafast frequency-agile terahertz devices using methylammonium lead halide perovskites

PubMed Central

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

2018-01-01

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

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

PubMed

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

2018-05-01

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

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

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

Correlated terahertz acoustic and electromagnetic emission in dynamically screened InGaN/GaN quantum wells

NASA Astrophysics Data System (ADS)

van Capel, P. J. S.; Turchinovich, D.; Porte, H. P.; Lahmann, S.; Rossow, U.; Hangleiter, A.; Dijkhuis, J. I.

2011-08-01

We investigate acoustic and electromagnetic emission from optically excited strained piezoelectric In0.2Ga0.8N/GaN multiple quantum wells (MQWs), using optical pump-probe spectroscopy, time-resolved Brillouin scattering, and THz emission spectroscopy. A direct comparison of detected acoustic signals and THz electromagnetic radiation signals demonstrates that transient strain generation in InGaN/GaN MQWs is correlated with electromagnetic THz generation, and both types of emission find their origin in ultrafast dynamical screening of the built-in piezoelectric field in the MQWs. The measured spectral intensity of the detected Brillouin signal corresponds to a maximum strain amplitude of generated acoustic pulses of 2%. This value coincides with the static lattice-mismatch-induced strain in In0.2Ga0.8N/GaN, demonstrating the total release of static strain in MQWs via impulsive THz acoustic emission. This confirms the ultrafast dynamical screening mechanism in MQWs as a highly efficient method for impulsive strain generation.

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

Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

PubMed Central

Canton, Sophie E.; Kjær, Kasper S.; Vankó, György; van Driel, Tim B.; Adachi, Shin-ichi; Bordage, Amélie; Bressler, Christian; Chabera, Pavel; Christensen, Morten; Dohn, Asmus O.; Galler, Andreas; Gawelda, Wojciech; Gosztola, David; Haldrup, Kristoffer; Harlang, Tobias; Liu, Yizhu; Møller, Klaus B.; Németh, Zoltán; Nozawa, Shunsuke; Pápai, Mátyás; Sato, Tokushi; Sato, Takahiro; Suarez-Alcantara, Karina; Togashi, Tadashi; Tono, Kensuke; Uhlig, Jens; Vithanage, Dimali A.; Wärnmark, Kenneth; Yabashi, Makina; Zhang, Jianxin; Sundström, Villy; Nielsen, Martin M.

2015-01-01

Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor–acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined. PMID:25727920

Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

DOE PAGES

Canton, Sophie E.; Kjær, Kasper S.; Vankó, György; ...

2015-03-02

Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor–acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances.more » Thus experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.« less

PREFACE: Ultrafast and nonlinear optics in carbon nanomaterials

NASA Astrophysics Data System (ADS)

Kono, Junichiro

2013-02-01

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

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

NASA Astrophysics Data System (ADS)

Sension, R. J.

2017-06-01

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

Ultrafast Spectroscopy of Proton-Coupled Electron Transfer (PCET) in Photocatalysis

DTIC Science & Technology

2016-07-08

AFRL-AFOSR-VA-TR-2016-0244 Ultrafast Spectroscopy of Proton-Coupled Electron Transfer (PCET) in Photocatalysis Jahan Dawlaty UNIVERSITY OF SOUTHERN...TITLE AND SUBTITLE Ultrafast Spectroscopy of Proton-Coupled Electron Transfer (PCET) in Photocatalysis 5a. CONTRACT NUMBER 5b. GRANT NUMBER FA9550...298 Back (Rev. 8/98) DISTRIBUTION A: Distribution approved for public release. Final Report: AFOSR YIP Grant FA9550-13-1-0128: Ultrafast Spectroscopy

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

NASA Astrophysics Data System (ADS)

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

2005-05-01

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

Ultrafast Laser Interaction Processes for LIBS and Other Sensing Technologies

DTIC Science & Technology

2013-04-05

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

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

PubMed Central

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

2015-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

Ultrafast Nanoimaging of the Photoinduced Phase Transition Dynamics in VO2.

PubMed

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

2016-05-11

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

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

PubMed

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

2017-10-17

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

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 and nonlinear surface-enhanced Raman spectroscopy.

PubMed

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

2016-04-21

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

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

NASA Astrophysics Data System (ADS)

Zhang, Chi; Wong, Kenneth K. Y.

2013-12-01

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

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

PubMed

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

2017-12-26

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

Proceedings of "Optical Probes of Dynamics in Complex Environments"

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

Sension, R; Tokmakoff, A

2008-04-01

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

Ultrafast photoelectron spectroscopy of small molecule organic films

NASA Astrophysics Data System (ADS)

Read, Kendall Laine

As research in the field of ultrafast optics has produced shorter and shorter pulses, at an ever-widening range of frequencies, ultrafast spectroscopy has grown correspondingly. In particular, ultrafast photoelectron spectroscopy allows direct observation of electrons in transient or excited states, regardless of the eventual relaxation mechanisms. High-harmonic conversion of 800nm, femtosecond, Ti:sapphire laser pulses allows excite/probe spectroscopy down into atomic core level states. To this end, an ultrafast, X-UV photoelectron spectroscopic system is described, including design considerations for the high-harmonic generation line, the time of flight detector, and the subsequent data collection electronics. Using a similar experimental setup, I have performed several ultrafast, photoelectron excited state decay studies at the IBM, T. J. Watson Research Center. All of the observed materials were electroluminescent thin film organics, which have applications as the emitter layer in organic light emitting devices. The specific materials discussed are: Alq, BAlq, DPVBi, and Alq doped with DCM or DMQA. Alq:DCM is also known to lase at low photoexcitation thresholds. A detailed understanding of the involved relaxation mechanisms is beneficial to both applications. Using 3.14 eV excite, and 26.7 eV probe, 90 fs laser pulses, we have observed the lowest unoccupied molecular orbital (LUMO) decay rate over the first 200 picoseconds. During this time, diffusion is insignificant, and all dynamics occur in the absence of electron transport. With excitation intensities in the range of 100μJ/cm2, we have modeled the Alq, BAlq, and DPVBi decays via bimolecular singlet-singlet annihilation. At similar excitations, we have modeled the Alq:DCM decay via Förster transfer, stimulated emission, and excimeric formation. Furthermore, the Alq:DCM occupied to unoccupied molecular orbital energy gap was seen to shrink as a function of excite-to-probe delay, in accordance with the expected relaxation within the excited states. Stable, shorter pulses allow finer temporal resolution and more efficient high-harmonic generation. This work therefore concludes by discussing a method for further shortening 25 femtosecond pulses via self-phase modulation, using filamentation in air and subsequent fiber channeling.

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

PubMed

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

2018-03-01

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

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

PubMed

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

2018-06-21

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

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

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

Luo, Liang; Wang, Jigang

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

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

DOE PAGES

Luo, Liang; Wang, Jigang

2016-01-01

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

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

PubMed

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

2011-10-01

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

Space-and-time resolved spectroscopy of single GaN nanowires

DOE PAGES

Upadhya, Prashanth C.; Martinez, Julio A.; Li, Qiming; ...

2015-06-30

Gallium nitridenanowires have garnered much attention in recent years due to their attractive optical and electrical properties. An understanding of carrier transport, relaxation, and recombination in these quasi-one-dimensional nanosystems is therefore important in optimizing them for various applications. We present ultrafast optical microscopic measurements on single GaNnanowires. Furthermore, our experiments, performed while varying the light polarization,excitation fluence, and position, give insight into the mechanisms governing carrier dynamics in these nanosystems.

Tunable Ultrafast Photon Source and Imaging System for Studying Carrier Dynamics in Graphene Devices

DTIC Science & Technology

2015-07-23

structure systems (for example of graphene and boron nitride ). Figure 2 shows the homebuilt Raman spectroscopy setup in our lab which uses two...pseudo-Dirac points in the band structure. In a run up to these studies, we have also developed a technique to optically image boron nitride flakes with...2) Dheeraj Golla, K. Chattrakun, K. Watanabe, T. Taniguchi, Brian J. LeRoy, Arvinder Sandhu, “Optical thickness determination of hexagonal boron

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

NASA Astrophysics Data System (ADS)

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

2017-05-01

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

Plasmonic Antennas for Optical Nanocrystallography and Femtosecond Spatio-Temporal Control

NASA Astrophysics Data System (ADS)

Berweger, Samuel

Controlling optical fields on nanometer length scales has been a long standing problem in optics, driven by the desire to image spatial inhomogeneities of condensed matter on the natural length scales of molecular, electronic, or lattice correlations. The concept of optical antennas based on plasmon resonant nanostructures has emerged as an attractive solution for concentrating and confining light to the nanoscale with a high degree of spatial confinement achieved in the evanescent field. This dissertation focuses on the fundamental characteristics of the antenna properties of plasmonic metal tips and their application for nanometer-resolved optical scanning probe spectroscopy and imaging. First this work demonstrates the extension of tip-enhanced Raman scattering (TERS) to optical nanocrystallography in order to study ferroelectric domain order by using the symmetry selective Raman selection rules for polar phonon modes in combination with the polarization-dependent TERS enhancement. After the derivation of the polar phonon TERS selection rules, ferroelectric domains arising from finite size effects within individual BaTiO3 nanorods are imaged. The second part of this work explores the fundamental characteristics and applications of adiabatic surface plasmon polariton (SPP) nanofocusing as an optical antenna for far- to near-field mode transformation. This process, resulting from the radius-dependent index of refraction experienced by SPP's propagating on tapered waveguides, is shown to result in a nanoconfined optical excitation at the apex of Au tips 10's of nm in size. To demonstrate the general application for background-free spectroscopy, adiabatic nanofocusing TERS is shown to improve contrast and sensitivity, and enables the extension to the near-IR spectral range. Lastly, due to the phase, wavelength, and amplitude independent nanofocusing mechanism, the independent and simultaneous nanometer-femtosecond spatio-temporal control of ultrafast pulses is possible. Combining the frequency domain shaping of optical transients with nanofocusing, we demonstrate the deterministic control of pulses as short as 16 fs and the generation of arbitrary waveforms at the tip apex. These results demonstrate the capability of these plasmonic optical antennas to not only generate enhanced optical fields for the study of matter on the nanoscale, but also to control ultrafast nano-optical excitations with applications for imaging and spectroscopy.

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

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.

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

PubMed

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

2013-08-02

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

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.

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

NASA Astrophysics Data System (ADS)

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

2017-09-01

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

Broadband extreme ultraviolet probing of transient gratings in vanadium dioxide

DOE PAGES

Sistrunk, Emily; Grilj, Jakob; Jeong, Jaewoo; ...

2015-02-11

Nonlinear spectroscopy in the extreme ultraviolet (EUV) and soft x-ray spectral range offers the opportunity for element selective probing of ultrafast dynamics using core-valence transitions (Mukamel et al., Acc. Chem. Res. 42, 553 (2009)). The study demonstrate a step on this path showing core-valence sensitivity in transient grating spectroscopy with EUV probing. We study the optically induced insulator-to-metal transition (IMT) of a VO 2 film with EUV diffraction from the optically excited sample. The VO 2 exhibits a change in the 3p-3d resonance of V accompanied by an acoustic response. Due to the broadband probing we are able to separatemore » the two features.« less

Efficient two-stage dual-beam noncollinear optical parametric amplifier

NASA Astrophysics Data System (ADS)

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

2018-06-01

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

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.

Transient GaAs plasmonic metasurfaces at terahertz frequencies

DOE PAGES

Yang, Yuanmu; Kamaraju, N.; Campione, Salvatore; ...

2016-12-09

Here we demonstrate the ultrafast formation of terahertz (THz) metasurfaces through all-optical creation of spatially modulated carrier density profiles in a deep-subwavelength GaAs film. The switch-on of the transient plasmon mode, governed by the GaAs effective electron mass and electron–phonon interactions, is revealed by structured-optical pump THz probe spectroscopy, on a time scale of 500 fs. By modulating the carrier density using different pump fluences, we observe a wide tuning of the electric dipole resonance of the transient GaAs metasurface from 0.5 THz to 1.7 THz. Furthermore, we numerically demonstrate that the metasurface presented here can be generalized to moremore » complex architectures for realizing functionalities such as perfect absorption, leading to a 30 dB modulation depth. In conclusion, the platform also provides a pathway to achieve ultrafast manipulation of infrared beams in the linear and, potentially, nonlinear regime.« less

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

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

Spectroscopic Studies of Carotenoid-to-Bacteriochlorophyll Energy Transfer in LHRC Photosynthetic Complex from Roseiflexus castenholzii

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

Niedzwiedzki, Dariusz; Collins, Aaron M.; LaFountain, Amy M.

Carotenoids present in the photosynthetic light-harvesting reaction center (LHRC) complex from chlorosome lacking filamentous anoxygenic phototroph, Roseiflexus castenholzii were purified and characterized for their photochemical properties. The LHRC from anaerobically grown cells contains five different carotenoids, methoxy-keto-myxocoxanthin, γ-carotene, and its three derivatives, whereas the LHRC from aerobically grown cells contains only three carotenoid pigments with methoxy-keto-myxocoxanthin being the dominant one. The spectroscopic properties and dynamics of excited singlet states of the carotenoids were studied by steady-state absorption, fluorescence and ultrafast time-resolved optical spectroscopy in organic solvent and in the intact LHRC complex. Time-resolved transient absorption spectroscopy performed in the near-infraredmore » (NIR) on purified carotenoids combined with steady-state absorption spectroscopy led to the precise determination of values of the energies of the S 1(2 1A g -) excited state. Global and single wavelength fitting of the ultrafast spectral and temporal data sets of the carotenoids in solvents and in the LHRC revealed the pathways of de-excitation of the carotenoid excited states.« less

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

PubMed

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

2017-06-14

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

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

NASA Astrophysics Data System (ADS)

Schilling, Daniel; Hertel, Tobias

2013-03-01

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

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

NASA Astrophysics Data System (ADS)

Sension, Roseanne

2015-03-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Dual comb generation from a mode-locked fiber laser with orthogonally polarized interlaced pulses.

PubMed

Akosman, Ahmet E; Sander, Michelle Y

2017-08-07

Ultra-high precision dual-comb spectroscopy traditionally requires two mode-locked, fully stabilized lasers with complex feedback electronics. We present a novel mode-locked operation regime in a thulium-holmium co-doped fiber laser, a frequency-halved state with orthogonally polarized interlaced pulses, for dual comb generation from a single source. In a linear fiber laser cavity, an ultrafast pulse train composed of co-generated, equal intensity and orthogonally polarized consecutive pulses at half of the fundamental repetition rate is demonstrated based on vector solitons. Upon optical interference of the orthogonally polarized pulse trains, two stable microwave RF beat combs are formed, effectively down-converting the optical properties into the microwave regime. These co-generated, dual polarization interlaced pulse trains, from one all-fiber laser configuration with common mode suppression, thus provide an attractive compact source for dual-comb spectroscopy, optical metrology and polarization entanglement measurements.

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

PubMed

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

2016-05-16

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

Ultrafast Laser Interaction Processes for Libs and Other Sensing Technologies

DTIC Science & Technology

2013-04-05

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

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

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

Applications of terahertz spectroscopy and imaging

NASA Astrophysics Data System (ADS)

Zhang, Cunlin; Mu, Kaijun

2009-07-01

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

Plasmon-Exciton Coupling Interaction for Surface Catalytic Reactions.

PubMed

Wang, Jingang; Lin, Weihua; Xu, Xuefeng; Ma, Fengcai; Sun, Mengtao

2018-05-01

In this review, we firstly reveal the physical principle of plasmon-exciton coupling interaction with steady absorption spectroscopy, and ultrafast transition absorption spectroscopy, based on the pump-prop technology. Secondly, we introduce the fabrication of electro-optical device of two-dimensional semiconductor-nanostructure noble metals hybrid, based on the plasmon-exciton coupling interactions. Thirdly, we introduce the applications of plasmon-exciton coupling interaction in the field of surface catalytic reactions. Lastly, the perspective of plasmon-exciton coupling interaction and applications closed this review. © 2018 The Chemical Society of Japan & Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

PubMed

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

2013-01-01

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

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

PubMed Central

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

2013-01-01

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

Unraveling shock-induced chemistry using ultrafast lasers

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

Moore, David Steven

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

Ultrafast carrier dynamics in GaN/InGaN multiple quantum wells nanorods

NASA Astrophysics Data System (ADS)

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

2018-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2016-10-01

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

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

PubMed

Stingel, Ashley M; Petersen, Poul B

2018-03-15

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

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

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

Chromatic effect in a novel THz generation scheme

NASA Astrophysics Data System (ADS)

Li, Bin; Zhang, Wenyan; Liu, Xiaoqing; Deng, Haixiao; Lan, Taihe; Liu, Bo; Liu, Jia; Wang, Xingtao; Zeng, Zhinan; Zhang, Lijian

2017-11-01

Deriving single or few cycle terahertz (THz) pulse by an intense femtosecond laser through cascaded optical rectification is a crucial technique in cutting-edge time-resolved spectroscopy to characterize micro-scale structures and ultrafast dynamics. Due to the broadband nature of the ultrafast driving laser, the chromatic effect limits the THz conversion efficiency in optical rectification crystals, especially for those implementing the pulse-front tilt scheme, e.g. lithium niobate (LN) crystal, has been prevalently used in the past decade. In this research we developed a brand new type of LN crystal utilizing Brewster coupling, and conducted systematically experimental and simulative investigation for the chromatic effect and multi-dimensionally entangled parameters in THz generation, predicting that an extreme conversion efficiency of ˜10% would be potentially achievable at the THz absorption coefficient of ˜0.5 cm-1. Moreover, we first discovered that the chirp of the driving laser plays a decisive role in the pulse-front tilt scheme, and the THz generation efficiency could be enhanced tremendously by applying an appropriate chirp.

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.

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

PubMed

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

2009-07-01

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

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

PubMed

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

2013-01-01

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

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

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

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

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

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

DOE PAGES

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

2017-10-17

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

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

PubMed

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

2014-09-21

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

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

PubMed

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

2016-06-27

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

The complete optical oscilloscope

NASA Astrophysics Data System (ADS)

Lei, Cheng; Goda, Keisuke

2018-04-01

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

Investigation of Energy Transfer Dynamics Between Target Contrast Agents and Prostate Cancer Cells Using Ultrafast Spectroscopy

DTIC Science & Technology

2012-05-01

morphometric comparison with clinically detected cancer in totally embedded specimens”, Hum. Pathol., 36, 646– 654 (2005). 20. Y. Pu, W. B. Wang...combination of optical spectroscopic investigations and fractal geometric analysis presents an intriguing possibility for development of a useful...prostate cancer. Morphometric analysis in whole-mount sections’’. Virchow Arch. 2000. 437: 625-634. 4. M. Chaplin. ‘‘Do we underestimate the importance

The Role of Electronic and Phononic Excitation in the Optical Response of Monolayer WS 2 after Ultrafast Excitation

DOE PAGES

Ruppert, Claudia; Chernikov, Alexey; Hill, Heather M.; ...

2017-01-06

We study transient changes of the optical response of WS 2 monolayers by femtosecond broadband pump–probe spectroscopy. Time-dependent absorption spectra are analyzed by tracking the line width broadening, bleaching, and energy shift of the main exciton resonance as a function of time delay after the excitation. Two main sources for the pump-induced changes of the optical response are identified. Specifically, we find an interplay between modifications induced by many-body interactions from photoexcited carriers and by the subsequent transfer of the excitation to the phonon system followed by cooling of the material through the heat transfer to the substrate.

The Role of Electronic and Phononic Excitation in the Optical Response of Monolayer WS 2 after Ultrafast Excitation

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

Ruppert, Claudia; Chernikov, Alexey; Hill, Heather M.

We study transient changes of the optical response of WS 2 monolayers by femtosecond broadband pump–probe spectroscopy. Time-dependent absorption spectra are analyzed by tracking the line width broadening, bleaching, and energy shift of the main exciton resonance as a function of time delay after the excitation. Two main sources for the pump-induced changes of the optical response are identified. Specifically, we find an interplay between modifications induced by many-body interactions from photoexcited carriers and by the subsequent transfer of the excitation to the phonon system followed by cooling of the material through the heat transfer to the substrate.

Effects of environmental conditions on the ultrafast carrier dynamics in graphene revealed by terahertz spectroscopy

NASA Astrophysics Data System (ADS)

Hafez, H. A.; Chai, X.; Sekine, Y.; Takamura, M.; Oguri, K.; Al-Naib, I.; Dignam, M. M.; Hibino, H.; Ozaki, T.

2017-04-01

A thorough understanding of the stability of graphene under ambient environmental conditions is essential for future graphene-based applications. In this paper, we study the effects of ambient temperature on the properties of monolayer graphene using terahertz time-domain spectroscopy as well as time-resolved terahertz spectroscopy enabled by an optical-pump/terahertz-probe technique. The observations show that graphene is extremely sensitive to the ambient environmental conditions and behaves differently depending on the sample preparation technique and the initial Fermi level. The analysis of the spectroscopic data is supported by van der Pauw and Hall effect measurements of the carrier mobility and carrier density at temperatures comparable to those tested in our THz spectroscopic experiments.

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

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

NASA Astrophysics Data System (ADS)

Kim, Jungho

2014-02-01

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

Synthesis and Characterization of Manganese Doped Silicon Nanoparticles

PubMed Central

Zhang, Xiaoming; Brynda, Marcin; Britt, R. David; Carroll, Elizabeth; Larsen, Delmar S.; Louie, Angelique Y.; Kauzlarich, Susan M.

2008-01-01

Mn doped Si nanoparticles have been synthesized via a low temperature solution route and characterize by X-ray powder diffraction, TEM, optical and emission spectroscopy and by EPR. The particle diameter was 4 nm and the surface was capped by octyl groups. 5% Mn doping resulted in a green emission with slightly lower quantum yield than undoped Si nanoparticles prepared by the same method. Mn2+ doped into the nanoparticle is confirmed by epr hyperfine and the charge carrier dynamics were probed by ultrafast transient absorption spectroscopy. Both techniques are consistent with Mn2+ on or close to the surface of the nanoparticle. PMID:17691792

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

PubMed

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

2011-04-26

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

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

NASA Astrophysics Data System (ADS)

Karasawa, Naoki

2018-04-01

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

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

NASA Astrophysics Data System (ADS)

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

2014-08-01

A series of layered molybdenum dichalcogenides, i.e., MoX2 (X = S, Se and Te), were prepared in cyclohexyl pyrrolidinone by a liquid-phase exfoliation technique. The high quality of the two-dimensional nanostructures was verified by transmission electron microscopy and absorption spectroscopy. Open- and closed-aperture Z-scans were employed to study the nonlinear absorption and nonlinear refraction of the MoX2 dispersions, respectively. All the three-layered nanostructures exhibit prominent ultrafast saturable absorption (SA) for both femtosecond (fs) and picosecond (ps) laser pulses over a broad wavelength range from the visible to the near infrared. While the dispersions treated with low-speed centrifugation (1500 rpm) have an SA response, and the MoS2 and MoSe2 dispersions after higher speed centrifugation (10 000 rpm) possess two-photon absorption for fs pulses at 1030 nm, which is due to the significant reduction of the average thickness of the nanosheets; hence, the broadening of band gap. In addition, all dispersions show obvious nonlinear self-defocusing for ps pulses at both 1064 nm and 532 nm, resulting from the thermally-induced nonlinear refractive index. The versatile ultrafast nonlinear properties imply a huge potential of the layered MoX2 semiconductors in the development of nanophotonic devices, such as mode-lockers, optical limiters, optical switches, etc.A series of layered molybdenum dichalcogenides, i.e., MoX2 (X = S, Se and Te), were prepared in cyclohexyl pyrrolidinone by a liquid-phase exfoliation technique. The high quality of the two-dimensional nanostructures was verified by transmission electron microscopy and absorption spectroscopy. Open- and closed-aperture Z-scans were employed to study the nonlinear absorption and nonlinear refraction of the MoX2 dispersions, respectively. All the three-layered nanostructures exhibit prominent ultrafast saturable absorption (SA) for both femtosecond (fs) and picosecond (ps) laser pulses over a broad wavelength range from the visible to the near infrared. While the dispersions treated with low-speed centrifugation (1500 rpm) have an SA response, and the MoS2 and MoSe2 dispersions after higher speed centrifugation (10 000 rpm) possess two-photon absorption for fs pulses at 1030 nm, which is due to the significant reduction of the average thickness of the nanosheets; hence, the broadening of band gap. In addition, all dispersions show obvious nonlinear self-defocusing for ps pulses at both 1064 nm and 532 nm, resulting from the thermally-induced nonlinear refractive index. The versatile ultrafast nonlinear properties imply a huge potential of the layered MoX2 semiconductors in the development of nanophotonic devices, such as mode-lockers, optical limiters, optical switches, etc. Electronic supplementary information (ESI) available: Electron scattering patterns from TEM characterizations of MX2 nanosheets; CA Z-scan results of graphene dispersions in the ps region. See DOI: 10.1039/c4nr02634a

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

PubMed

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

2010-09-27

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

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

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

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

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

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

PubMed

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

2018-01-28

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

Free-electron laser spectroscopy in biology, medicine, and materials science; Proceedings of the Meeting, Los Angeles, CA, Jan. 22, 1993

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

Schwettman, H.A.

1993-01-01

Various papers on FEL spectroscopy in biology, medicine, and materials science are presented. Individual topics addressed include: Vanderbilt University FEL Center, FIR FEL facility at the University of California/Santa Barbara, FEL research facilities and opportunities at Duke, facilities at the Stanford Picosecond FEL Center, FIR nonlinear response of electrons in semiconductor nanostructures, FIR harmonic generation from semiconductor heterostructures, intrinsic response times of double-barrier resonant tunneling diodes at tetrahertz frequencies, semiconductor spectroscopy and ablation processes with the Vanderbilt FEL. Also discussed are: picosecond nonlinear optics in semiconductor quantum wells with the SCA FEL, excitation spectroscopy of thin-film disordered semiconductors, biophysical applicationmore » of FELs, FEL investigation of energy transfer in condensed phase systems, probing protein photochemistry and dynamics with ultrafast infrared spectroscopy, plasma ablation of hard tissues by FEL, FEL irradiation of the cornea.« less

Steering optical comb frequencies by rotating the polarization state

NASA Astrophysics Data System (ADS)

Zhang, Yanyan; Zhang, Xiaofei; Yan, Lulu; Zhang, Pan; Rao, Bingjie; Han, Wei; Guo, Wenge; Zhang, Shougang; Jiang, Haifeng

2017-12-01

Optical frequency combs, with precise control of repetition rate and carrier-envelope-offset frequency, have revolutionized many fields, such as fine optical spectroscopy, optical frequency standards, ultra-fast science research, ultra-stable microwave generation and precise ranging measurement. However, existing high bandwidth frequency control methods have small dynamic range, requiring complex hybrid control techniques. To overcome this limitation, we develop a new approach, where a home-made intra-cavity electro-optic modulator tunes polarization state of laser signal rather than only optical length of the cavity, to steer frequencies of a nonlinear-polarization-rotation mode-locked laser. By taking advantage of birefringence of the whole cavity, this approach results in not only broadband but also relative large-dynamic frequency control. Experimental results show that frequency control dynamic range increase at least one order in comparison with the traditional intra-cavity electro-optic modulator technique. In additional, this technique exhibits less side-effect than traditional frequency control methods.

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

NASA Astrophysics Data System (ADS)

Nurmohammadi, Tofiq; Abbasian, Karim; Yadipour, Reza

2018-05-01

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

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

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

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

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

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.

Room-temperature ultrafast nonlinear spectroscopy of a single molecule

NASA Astrophysics Data System (ADS)

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

2018-01-01

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

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

PubMed

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

2017-08-03

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

Ultrafast control and monitoring of material properties using terahertz pulses

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

Bowlan, Pamela Renee

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

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

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

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

Sarkar, Ketaki; Mukherjee, Souvik; Wiederrecht, Gary

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

Ultrafast hydrogen bond dynamics and partial electron transfer after photoexcitation of diethyl ester of 7-(diethylamino)-coumarin-3-phosphonic acid and its benzoxaphosphorin analog.

PubMed

Wagner, M S; Ilieva, E D; Petkov, P St; Nikolova, R D; Kienberger, R; Iglev, H

2015-04-21

The solvation dynamics after optical excitation of two phosphono-substituted coumarin derivatives dissolved in various solutions are studied by fluorescence up-conversion spectroscopy and quantum chemical simulations. The Kamlet-Taft analysis of the conventional absorption and emission spectra suggests weakening of the solvent-solute H-bonds upon optical excitation, which is in contrast to the results gained by the quantum simulations and earlier studies reported for coumarin derivatives without phosphono groups. The simulations give evidence that the solvent reorganisation around the excited fluorophore leads to partial electron transfer to the first solvation shell. The process occurs on a timescale between 1 and 10 ps depending on the solvent polarity and leads to a fast decay of the time-resolved emission signal. Using the ultrafast spectral shift of the time-dependent fluorescence we estimated the relaxation time of the H-bonds in the electronically excited state to be about 0.6 ps in water, 1.5 ps in ethanol and 2.8 ps in formamide.

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

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

DOE PAGES

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

2018-01-04

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

Ultrafast carrier dynamics in the large-magnetoresistance material WTe 2

DOE PAGES

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

2015-10-07

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

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

PubMed

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

2017-02-01

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

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

PubMed

Turton, David A; Wynne, Klaas

2008-04-21

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

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).

Apparatus and method for characterizing ultrafast polarization varying optical pulses

DOEpatents

Smirl, Arthur; Trebino, Rick P.

1999-08-10

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

Real-Time Visualization of Active Species in a Single-Site Metal–Organic Framework Photocatalyst

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

Yang, Sizhuo; Pattengale, Brian; Lee, Sungsik

In this work, we report a new single-site photocatalyst (Co-Ru-UIO- 67(bpy)) based on a metal-organic framework platform with incorporated molecular photosensitizer and catalyst. We show that this catalyst not only demonstrates exceptional activity for light-driven H2 production but also can be recycled without loss of activity. Using the combination of optical transient absorption spectroscopy and in situ X-ray absorption spectroscopy, we not only captured the key CoI intermediate species formed after ultrafast charge transfer from the incorporated photosensitizer but also identified the rate-limiting step in the catalytic cycle, providing insight into the catalysis mechanism of these single-site metal-organic framework photocatalysts.

Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.

PubMed

Loh, Zhi-Heng; Khalil, Munira; Correa, Raoul E; Santra, Robin; Buth, Christian; Leone, Stephen R

2007-04-06

Femtosecond high-order harmonic transient absorption spectroscopy is used to resolve the complete |j,m quantum state distribution of Xe+ produced by optical strong-field ionization of Xe atoms at 800 nm. Probing at the Xe N4/5 edge yields a population distribution rhoj,|m| of rho3/2,1/2ratiorho1/2,1/2ratiorho3/2,3/2=75+/-6 :12+/-3 :13+/-6%. The result is compared to a tunnel ionization calculation with the inclusion of spin-orbit coupling, revealing nonadiabatic ionization behavior. The sub-50-fs time resolution paves the way for tabletop extreme ultraviolet absorption probing of ultrafast dynamics.

Apparatus and method for characterizing ultrafast polarization varying optical pulses

DOEpatents

Smirl, A.; Trebino, R.P.

1999-08-10

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

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.

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

PubMed

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

2011-03-14

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

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

NASA Astrophysics Data System (ADS)

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

2015-10-01

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

Time-domain separation of optical properties from structural transitions in resonantly bonded materials.

PubMed

Waldecker, Lutz; Miller, Timothy A; Rudé, Miquel; Bertoni, Roman; Osmond, Johann; Pruneri, Valerio; Simpson, Robert E; Ernstorfer, Ralph; Wall, Simon

2015-10-01

The extreme electro-optical contrast between crystalline and amorphous states in phase-change materials is routinely exploited in optical data storage and future applications include universal memories, flexible displays, reconfigurable optical circuits, and logic devices. Optical contrast is believed to arise owing to a change in crystallinity. Here we show that the connection between optical properties and structure can be broken. Using a combination of single-shot femtosecond electron diffraction and optical spectroscopy, we simultaneously follow the lattice dynamics and dielectric function in the phase-change material Ge2Sb2Te5 during an irreversible state transformation. The dielectric function changes by 30% within 100 fs owing to a rapid depletion of electrons from resonantly bonded states. This occurs without perturbing the crystallinity of the lattice, which heats with a 2-ps time constant. The optical changes are an order of magnitude larger than those achievable with silicon and present new routes to manipulate light on an ultrafast timescale without structural changes.

Modelling multi-pulse population dynamics from ultrafast spectroscopy.

PubMed

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

2011-03-21

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

Modelling Multi-Pulse Population Dynamics from Ultrafast Spectroscopy

PubMed Central

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

2011-01-01

Current advanced laser, optics and electronics technology allows sensitive recording of molecular dynamics, from single resonance to multi-colour and multi-pulse experiments. Extracting the occurring (bio-) physical relevant pathways via global analysis of experimental data requires a systematic investigation of connectivity schemes. Here we present a Matlab-based toolbox for this purpose. The toolbox has a graphical user interface which facilitates the application of different reaction models to the data to generate the coupled differential equations. Any time-dependent dataset can be analysed to extract time-independent correlations of the observables by using gradient or direct search methods. Specific capabilities (i.e. chirp and instrument response function) for the analysis of ultrafast pump-probe spectroscopic data are included. The inclusion of an extra pulse that interacts with a transient phase can help to disentangle complex interdependent pathways. The modelling of pathways is therefore extended by new theory (which is included in the toolbox) that describes the finite bleach (orientation) effect of single and multiple intense polarised femtosecond pulses on an ensemble of randomly oriented particles in the presence of population decay. For instance, the generally assumed flat-top multimode beam profile is adapted to a more realistic Gaussian shape, exposing the need for several corrections for accurate anisotropy measurements. In addition, the (selective) excitation (photoselection) and anisotropy of populations that interact with single or multiple intense polarised laser pulses is demonstrated as function of power density and beam profile. Using example values of real world experiments it is calculated to what extent this effectively orients the ensemble of particles. Finally, the implementation includes the interaction with multiple pulses in addition to depth averaging in optically dense samples. In summary, we show that mathematical modelling is essential to model and resolve the details of physical behaviour of populations in ultrafast spectroscopy such as pump-probe, pump-dump-probe and pump-repump-probe experiments. PMID:21445294

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

PubMed

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

2016-10-01

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

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

DOE PAGES

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

2017-11-28

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

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

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

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

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

Overview of selected seminal optical science and photonics processes in nature

NASA Astrophysics Data System (ADS)

Alfano, Robert R.

2016-03-01

This presentation gives an overview on some of seminal research in optical science, condensed matter physics, biophysics, biology, biomedical, nonlinear optics, and structure light propagation and interactions at CCNY and GTE Labs over past 46 years. The advent of ultrafast laser pulses with picosecond and femtosecond pulses and optical spectroscopy (label free native fluorescence and Raman) has led to unravel some of mysteries in the molecular world leading to breakthroughs in various areas of science and medicine. The following topics are discussed: white light continuum called now Supercontinuum (SC); first direct measurement of Optical Phonon's lifetimes; first observation of creation of daughter vibrations in time from excited mother vibration in liquids; first direct measurement of creation and decay of Spin Angular Momentum of electrons in GaAs where picosecond Circular Polarized Light carrying Optical Spin Angular Momentum is generated; Pulse break up into ballistic, snake and diffusive components in scattering media such as um beads and tissues; and use of optical spectroscopy for first cancer detection in label free tissues. Most recently, advances in Biomedical Optics showed that Tryptophan as a key biomarker for aggressive cancers; there are three new optical windows with the Golden window #3 the best for penetrating tissue from 1600 nm to 1800 nm; Complex light with OAM offers potential deeper tissue penetration and Resonance Raman excited using magic 532 nm wavelength in tissues.

Using ultrashort terahertz pulses to directly probe spin dynamics in insulating antiferromagnets

NASA Astrophysics Data System (ADS)

Bowlan, P.; Trugman, S. A.; Yarotski, D. A.; Taylor, A. J.; Prasankumar, R. P.

2018-05-01

Terahertz pulses are a direct and general probe of ultrafast spin dynamics in insulating antiferromagnets (AFM). This is shown by using optical-pump, THz-probe spectroscopy to directly track AFM spin dynamics in the hexagonal multiferroic HoMnO3 and the orthorhombic multiferroic TbMnO3. Our studies show that despite the different structural and spin orders in these materials, THz pulses can unambiguously resolve spin dynamics after optical photoexcitation. We believe that this approach is quite general and can be applied to a broad range of materials with different AFM spin alignments, providing a novel non-contact approach for probing AFM order with femtosecond temporal resolution.

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.

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

PubMed

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

2011-03-01

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

Compressive sensing for single-shot two-dimensional coherent spectroscopy

NASA Astrophysics Data System (ADS)

Harel, E.; Spencer, A.; Spokoyny, B.

2017-02-01

In this work, we explore the use of compressive sensing for the rapid acquisition of two-dimensional optical spectra that encodes the electronic structure and ultrafast dynamics of condensed-phase molecular species. Specifically, we have developed a means to combine multiplexed single-element detection and single-shot and phase-resolved two-dimensional coherent spectroscopy. The method described, which we call Single Point Array Reconstruction by Spatial Encoding (SPARSE) eliminates the need for costly array detectors while speeding up acquisition by several orders of magnitude compared to scanning methods. Physical implementation of SPARSE is facilitated by combining spatiotemporal encoding of the nonlinear optical response and signal modulation by a high-speed digital micromirror device. We demonstrate the approach by investigating a well-characterized cyanine molecule and a photosynthetic pigment-protein complex. Hadamard and compressive sensing algorithms are demonstrated, with the latter achieving compression factors as high as ten. Both show good agreement with directly detected spectra. We envision a myriad of applications in nonlinear spectroscopy using SPARSE with broadband femtosecond light sources in so-far unexplored regions of the electromagnetic spectrum.

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

DOE PAGES

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

2017-06-23

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

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

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

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

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

Ultrafast transient photocarrier dynamics of the bulk-insulating topological insulator B i1.5S b0.5T e1.7S e1.3

NASA Astrophysics Data System (ADS)

Choi, Young Gwan; Zhung, Chan June; Park, Sun-Hee; Park, Joonbum; Kim, Jun Sung; Kim, Seongheun; Park, Jaehun; Lee, J. S.

2018-02-01

Using optical-pump terahertz-probe spectroscopy, we investigated an ultrafast photocarrier relaxation behavior in a B i1.5S b0.5T e1.7S e1.3 (BSTS) single crystal, which is one of the most bulk-insulating topological insulators. Compared to n -type bulk-metallic B i2S e3 , we found that BSTS endows distinct behaviors in its photocarrier dynamics; the relaxation time turns out to be an order of magnitude longer, and the transient conductance spectrum exhibits a nonlinear increase as a function of the pumping power. Also, we observed an abrupt reduction of the photocarrier scattering rate in several picoseconds after the initial photoexcitation. We discuss these intriguing experimental observations based on a bulk-to-surface carrier injection assisted by the built-in electric field near the surface and electron-phonon scattering.

Polarization-dependent force driving the Eg mode in bismuth under optical excitation: comparison of first-principles theory with ultra-fast x-ray experiments

NASA Astrophysics Data System (ADS)

Fahy, Stephen; Murray, Eamonn

2015-03-01

Using first principles electronic structure methods, we calculate the induced force on the Eg (zone centre transverse optical) phonon mode in bismuth immediately after absorption of a ultrafast pulse of polarized light. To compare the results with recent ultra-fast, time-resolved x-ray diffraction experiments, we include the decay of the force due to carrier scattering, as measured in optical Raman scattering experiments, and simulate the optical absorption process, depth-dependent atomic driving forces, and x-ray diffraction in the experimental geometry. We find excellent agreement between the theoretical predictions and the observed oscillations of the x-ray diffraction signal, indicating that first-principles theory of optical absorption is well suited to the calculation of initial atomic driving forces in photo-excited materials following ultrafast excitation. This work is supported by Science Foundation Ireland (Grant No. 12/IA/1601) and EU Commission under the Marie Curie Incoming International Fellowships (Grant No. PIIF-GA-2012-329695).

Method and apparatus for two-dimensional spectroscopy

DOEpatents

DeCamp, Matthew F.; Tokmakoff, Andrei

2010-10-12

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

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

NASA Astrophysics Data System (ADS)

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

2018-07-01

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

Near-field infrared vibrational dynamics and tip-enhanced decoherence.

PubMed

Xu, Xiaoji G; Raschke, Markus B

2013-04-10

Ultrafast infrared spectroscopy can reveal the dynamics of vibrational excitations in matter. In its conventional far-field implementation, however, it provides only limited insight into nanoscale sample volumes due to insufficient spatial resolution and sensitivity. Here, we combine scattering-scanning near-field optical microscopy (s-SNOM) with femtosecond infrared vibrational spectroscopy to characterize the coherent vibrational dynamics of a nanoscopic ensemble of C-F vibrational oscillators of polytetrafluoroethylene (PTFE). The near-field mode transfer between the induced vibrational molecular coherence and the metallic scanning probe tip gives rise to a tip-mediated radiative IR emission of the vibrational free-induction decay (FID). By increasing the tip–sample coupling, we can enhance the vibrational dephasing of the induced coherent vibrational polarization and associated IR emission, with dephasing times up to T2(NF) is approximately equal to 370 fs in competition against the intrinsic far-field lifetime of T2(FF) is approximately equal to 680 fs as dominated by nonradiative damping. Near-field antenna-coupling thus provides for a new way to modify vibrational decoherence. This approach of ultrafast s-SNOM enables the investigation of spatiotemporal dynamics and correlations with nanometer spatial and femtosecond temporal resolution.

Ultrafast Carrier dynamics of InxGa1-xN nanostructures grown directly on Si(111)

NASA Astrophysics Data System (ADS)

Kumar, Praveen; Devi, Pooja; Rodriguez⁠, P. E. D. S.; Kumar, Manish; Shivling, V. D.; Noetzel, Richard; Sharma, Chhavi; Sinha, R. K.; Kumar, Mahesh

2018-05-01

We show a flux dependence changes in structural, optical and electronic properties of InxGa1-xN nanostructures (NSs) namely nanocolumns (NCs), nanoflakes (NFs) and nanowall network (NWN) grown directly on Si(111) surface. Field emission scanning electron microscopy (FESEM) images were recorded to see morphological changes from NFs to NCs and NWNc etc, while high-resolution X-ray diffraction (HRXRD) ω-2θ scans were used to determine In incorporation. The maximum In incorporation was observed to be 20, 33 and 38% for the sharp transition from NFs to NCs and NWNs, respectively. The charge carrier dynamics of these grown NSs were probed using Ultrafast Femtosecond Transient Absorption Spectroscopy (UFTAS) with excitation at 350 nm pump wavelength. The UFTAS studies show the comparative charge carriers dynamics of the NWS, NCs and NFs. The charge carrier studies show a higher lifetime in NWNs as compare to NCs and NFs. Further, to examine electronic structure and level of degeneracy of these NSs, core-level and valence band spectra were analyzed by X-ray photoelectron spectroscopy (XPS), which manifest the upward band bending ranging from 0.2 eV to 0.4 eV.

Through a Window, Brightly: A Review of Selected Nanofabricated Thin-Film Platforms for Spectroscopy, Imaging, and Detection.

PubMed

Dwyer, Jason R; Harb, Maher

2017-09-01

We present a review of the use of selected nanofabricated thin films to deliver a host of capabilities and insights spanning bioanalytical and biophysical chemistry, materials science, and fundamental molecular-level research. We discuss approaches where thin films have been vital, enabling experimental studies using a variety of optical spectroscopies across the visible and infrared spectral range, electron microscopies, and related techniques such as electron energy loss spectroscopy, X-ray photoelectron spectroscopy, and single molecule sensing. We anchor this broad discussion by highlighting two particularly exciting exemplars: a thin-walled nanofluidic sample cell concept that has advanced the discovery horizons of ultrafast spectroscopy and of electron microscopy investigations of in-liquid samples; and a unique class of thin-film-based nanofluidic devices, designed around a nanopore, with expansive prospects for single molecule sensing. Free-standing, low-stress silicon nitride membranes are a canonical structural element for these applications, and we elucidate the fabrication and resulting features-including mechanical stability, optical properties, X-ray and electron scattering properties, and chemical nature-of this material in this format. We also outline design and performance principles and include a discussion of underlying material preparations and properties suitable for understanding the use of alternative thin-film materials such as graphene.

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

NASA Astrophysics Data System (ADS)

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

2017-10-01

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

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

PubMed

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

2018-02-27

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

Linear and nonlinear frequency- and time-domain spectroscopy with multiple frequency combs.

PubMed

Bennett, Kochise; Rouxel, Jeremy R; Mukamel, Shaul

2017-09-07

Two techniques that employ equally spaced trains of optical pulses to map an optical high frequency into a low frequency modulation of the signal that can be detected in real time are compared. The development of phase-stable optical frequency combs has opened up new avenues to metrology and spectroscopy. The ability to generate a series of frequency spikes with precisely controlled separation permits a fast, highly accurate sampling of the material response. Recently, pairs of frequency combs with slightly different repetition rates have been utilized to down-convert material susceptibilities from the optical to microwave regime where they can be recorded in real time. We show how this one-dimensional dual comb technique can be extended to multiple dimensions by using several combs. We demonstrate how nonlinear susceptibilities can be quickly acquired using this technique. In a second class of techniques, sequences of ultrafast mode locked laser pulses are used to recover pathways of interactions contributing to nonlinear susceptibilities by using a photo-acoustic modulation varying along the sequences. We show that these techniques can be viewed as a time-domain analog of the multiple frequency comb scheme.

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

Chen, R. Y.; Zhang, S. J.; Bauer, E. D.

We report optical spectroscopy and ultrafast pump-probe measurements on the antiferromagnetic heavy-fermion compound CePt 2 In 7 , a member showing stronger two dimensionality than other compounds in the CeIn 3 -derived heavy-fermion family. Here, we identify clear and typical hybridization spectral structures at low temperature from the two different spectroscopy probes. But, the strength and related energy scale of the hybridization are much weaker and smaller than that in the superconducting compounds CeCoIn 5 and CeIrIn 5 . The features are more similar to observations on the antiferromagnetic compounds CeIn 3 and CeRhIn 5 in the same family. Ourmore » results clearly indicate that the Kondo interaction and hybridizations exist in the antiferromagnetic compounds but with weaker strength.« less

Picosecond Transient Photoconductivity in Functionalized Pentacene Molecular Crystals Probed by Terahertz Pulse Spectroscopy

NASA Astrophysics Data System (ADS)

Hegmann, F. A.; Tykwinski, R. R.; Lui, K. P.; Bullock, J. E.; Anthony, J. E.

2002-11-01

We have measured transient photoconductivity in functionalized pentacene molecular crystals using ultrafast optical pump-terahertz probe techniques. The single crystal samples were excited using 800nm, 100fs pulses, and the change in transmission of time-delayed, subpicosecond terahertz pulses was used to probe the photoconducting state over a temperature range from 10 to 300K. A subpicosecond rise in photoconductivity is observed, suggesting that mobile carriers are a primary photoexcitation. At times longer than 4ps, a power-law decay is observed consistent with dispersive transport.

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

NASA Astrophysics Data System (ADS)

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

2016-09-01

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

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

PubMed

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

2016-09-01

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

Ultrafast 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

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

NASA Astrophysics Data System (ADS)

Kim, Jungho

2013-11-01

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

Ultrafast 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.

Theoretical Investigation of Device Aspects of Semiconductor Superlattices.

DTIC Science & Technology

1983-09-01

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

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

PubMed

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

2016-05-01

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

Watching the dynamics of electrons and atoms at work in solar energy conversion.

PubMed

Canton, S E; Zhang, X; Liu, Y; Zhang, J; Pápai, M; Corani, A; Smeigh, A L; Smolentsev, G; Attenkofer, K; Jennings, G; Kurtz, C A; Li, F; Harlang, T; Vithanage, D; Chabera, P; Bordage, A; Sun, L; Ott, S; Wärnmark, K; Sundström, V

2015-01-01

The photochemical reactions performed by transition metal complexes have been proposed as viable routes towards solar energy conversion and storage into other forms that can be conveniently used in our everyday applications. In order to develop efficient materials, it is necessary to identify, characterize and optimize the elementary steps of the entire process on the atomic scale. To this end, we have studied the photoinduced electronic and structural dynamics in two heterobimetallic ruthenium-cobalt dyads, which belong to the large family of donor-bridge-acceptor systems. Using a combination of ultrafast optical and X-ray absorption spectroscopies, we can clock the light-driven electron transfer processes with element and spin sensitivity. In addition, the changes in local structure around the two metal centers are monitored. These experiments show that the nature of the connecting bridge is decisive for controlling the forward and the backward electron transfer rates, a result supported by quantum chemistry calculations. More generally, this work illustrates how ultrafast optical and X-ray techniques can disentangle the influence of spin, electronic and nuclear factors on the intramolecular electron transfer process. Finally, some implications for further improving the design of bridged sensitizer-catalysts utilizing the presented methodology are outlined.

High-speed laser-launched flyer impacts studied with ultrafast photography and velocimetry

DOE PAGES

Banishev, Alexandr A.; Shaw, William L.; Bassett, Will P.; ...

2016-02-16

Pulsed lasers can launch thin metal foils at km s -1, but for precision measurements in shock compression science and shock wave spectroscopy, where one-dimensional shock compression is vital, flyer plate impacts with targets must have a high degree of flatness and minimal tilt, and the flyer speeds and impact times at the target must be highly reproducible. We have developed an apparatus that combines ultrafast stroboscopic optical microscopy with photon Doppler velocimetry to study impacts of laser-launched Al and Cu flyer plates with flat, transparent glass targets. The flyer plates were 0.5 mm in diameter, and ranged from 12-100more » μm thick, with flyer speeds up to 6.25 km s -1. The velocity variations over 30-60 launches from the same flyer plate optic can be as low as 0.6%, and the impact time variations can be as low as 0.8 ns. Stroboscopic image streams (reconstructed movies) show uniform, flat impacts with a glass target. As a result, these stroboscopic images can be used to estimate the tilt in the flyer-target impact to be <1mrad.« less

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

NASA Astrophysics Data System (ADS)

Torjesen, Alyssa; Istfan, Raeef; Roblyer, Darren

2017-03-01

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

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

PubMed Central

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

2015-01-01

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

Discrete decoding based ultrafast multidimensional nuclear magnetic resonance spectroscopy

NASA Astrophysics Data System (ADS)

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

2015-07-01

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

Stimulated Raman spectroscopy and nanoscopy of molecules using near field photon induced forces without resonant electronic enhancement gain

NASA Astrophysics Data System (ADS)

Tamma, Venkata Ananth; Huang, Fei; Nowak, Derek; Kumar Wickramasinghe, H.

2016-06-01

We report on stimulated Raman spectroscopy and nanoscopy of molecules, excited without resonant electronic enhancement gain, and recorded using near field photon induced forces. Photon-induced interaction forces between the sharp metal coated silicon tip of an Atomic Force Microscope (AFM) and a sample resulting from stimulated Raman excitation were detected. We controlled the tip to sample spacing using the higher order flexural eigenmodes of the AFM cantilever, enabling the tip to come very close to the sample. As a result, the detection sensitivity was increased compared with previous work on Raman force microscopy. Raman vibrational spectra of azobenzene thiol and l-phenylalanine were measured and found to agree well with published results. Near-field force detection eliminates the need for far-field optical spectrometer detection. Recorded images show spatial resolution far below the optical diffraction limit. Further optimization and use of ultrafast pulsed lasers could push the detection sensitivity towards the single molecule limit.

Stimulated Raman spectroscopy and nanoscopy of molecules using near field photon induced forces without resonant electronic enhancement gain

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

Tamma, Venkata Ananth; Huang, Fei; Kumar Wickramasinghe, H., E-mail: hkwick@uci.edu

We report on stimulated Raman spectroscopy and nanoscopy of molecules, excited without resonant electronic enhancement gain, and recorded using near field photon induced forces. Photon-induced interaction forces between the sharp metal coated silicon tip of an Atomic Force Microscope (AFM) and a sample resulting from stimulated Raman excitation were detected. We controlled the tip to sample spacing using the higher order flexural eigenmodes of the AFM cantilever, enabling the tip to come very close to the sample. As a result, the detection sensitivity was increased compared with previous work on Raman force microscopy. Raman vibrational spectra of azobenzene thiol andmore » l-phenylalanine were measured and found to agree well with published results. Near-field force detection eliminates the need for far-field optical spectrometer detection. Recorded images show spatial resolution far below the optical diffraction limit. Further optimization and use of ultrafast pulsed lasers could push the detection sensitivity towards the single molecule limit.« less

Optical tuning of electronic valleys (Conference Presentation)

NASA Astrophysics Data System (ADS)

Sie, Edbert J.; Gedik, Nuh

2017-02-01

Monolayer transition-metal dichalcogenides such as MoS2 and WS2 are prime examples of atomically thin semiconducting crystals that exhibit remarkable electronic and optical properties. They have a pair of valleys that can serve as a new electronic degree of freedom, and these valleys obey optical selection rules with circularly polarized light. Here, we discuss how ultrafast laser pulses can be used to tune their energy levels in a controllable valley-selective manner. The energy tunability is extremely large, comparable to what would be obtained using a hundred Tesla of magnetic field. We will also show that such valley tunability can be performed while we effectively manipulate the valley selection rules. Finally, we will explore the prospect of using this technique through photoemission spectroscopy to create a new phase of matter called a valley Floquet topological insulator.

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.

Ultrafast X-Ray Spectroscopy of Conical Intersections

NASA Astrophysics Data System (ADS)

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

2018-06-01

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

Optical properties of transiently-excited semiconductor hyperbolic metamaterials

DOE PAGES

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

2015-10-02

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

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

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

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

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

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

PubMed

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

2017-08-21

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

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

PubMed

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

2018-03-01

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

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

NASA Astrophysics Data System (ADS)

Kim, Jungho; Yu, Bong-Ahn

2015-03-01

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

The dependence of the ultrafast relaxation kinetics of the S2 and S1 states in β-carotene homologs and lycopene on conjugation length studied by femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies

NASA Astrophysics Data System (ADS)

Kosumi, Daisuke; Fujiwara, Masazumi; Fujii, Ritsuko; Cogdell, Richard J.; Hashimoto, Hideki; Yoshizawa, Masayuki

2009-06-01

The ultrafast relaxation kinetics of all-trans-β-carotene homologs with varying numbers of conjugated double bonds n(n =7-15) and lycopene (n =11) has been investigated using femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies, both carried out under identical excitation conditions. The nonradiative relaxation rates of the optically allowed S2(1Bu+1) state were precisely determined by the time-resolved fluorescence. The kinetics of the optically forbidden S1(2Ag-1) state were observed by the time-resolved absorption measurements. The dependence of the S1 relaxation rates upon the conjugation length is adequately described by application of the energy gap law. In contrast to this, the nonradiative relaxation rates of S2 have a minimum at n =9 and show a reverse energy gap law dependence for values of n above 11. This anomalous behavior of the S2 relaxation rates can be explained by the presence of an intermediate state (here called the Sx state) located between the S2 and S1 states at large values of n (such as n =11). The presence of such an intermediate state would then result in the following sequential relaxation pathway S2→Sx→S1→S0. A model based on conical intersections between the potential energy curves of these excited singlet states can readily explain the measured relationships between the decay rates and the energy gaps.

Femtosecond timing measurement and control using ultrafast organic thin films

NASA Astrophysics Data System (ADS)

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

2003-12-01

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

Material processing with fiber based ultrafast pulse delivery

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

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

PubMed

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

2017-04-03

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

Ultrafast Unzipping of a Beta-Hairpin Peptide

NASA Astrophysics Data System (ADS)

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

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

The Ultrafast Wolff Rearrangement in the Gas Phase

NASA Astrophysics Data System (ADS)

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

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

Microresonator-Based Optical Frequency Combs: A Time Domain Perspective

DTIC Science & Technology

2016-04-19

optics; ultrafast optics 16. SECURITY CLASSIFICATION OF: 17. LIMITATION OF ABSTRACT 18. NUMBER OF PAGES 19a. NAME OF RESPONSIBLE PERSON a...generation at frequency spacings down to 25 GHz, in the range where convenient electronic detection is possible. (c) Our best Purdue microrings had...time domain measurements of the generated combs, leading to observation of novel, ultrafast dark pulse waveforms, have introduced new structures such

40-Gbit/s all-optical circulating shift register with an inverter.

PubMed

Hall, K L; Donnelly, J P; Groves, S H; Fennelly, C I; Bailey, R J; Napoleone, A

1997-10-01

We report what is believed to be the first demonstration of an all-optical circulating shift register using an ultrafast nonlinear interferometer with a polarization-insensitive semiconductor optical amplifier as the nonlinear switching element. The device operates at 40 Gbits/s, to our knowledge the highest speed demonstrated to date. Also, the demonstration proves the cascadability of the ultrafast nonlinear interferometric switch.

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

NASA Astrophysics Data System (ADS)

Liu, Xiang; Beckwitt, Kale; Wise, Frank

2000-05-01

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

Photon-assisted electron energy loss spectroscopy and ultrafast imaging.

PubMed

Howie, Archie

2009-08-01

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

Ultrafast quantum control of ionization dynamics in krypton.

PubMed

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

2018-02-19

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

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

NASA Astrophysics Data System (ADS)

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

2017-02-01

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

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

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

DOE PAGES

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

2015-03-02

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

Large-area tungsten disulfide for ultrafast photonics.

PubMed

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

2017-02-02

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

3D microstructuring inside glass by ultrafast laser

NASA Astrophysics Data System (ADS)

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

2012-01-01

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

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

PubMed

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

2014-08-11

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

Recent advances in multidimensional ultrafast spectroscopy

NASA Astrophysics Data System (ADS)

Oliver, Thomas A. A.

2018-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2005-01-01

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

Recent advances in multidimensional ultrafast spectroscopy

PubMed Central

2018-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-09-01

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

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.

Towards Direct Measurement of Ultrafast Vibrational Energy Flow in Proteins

NASA Astrophysics Data System (ADS)

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

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

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.

Femtosecond characterization of vibrational optical activity of chiral molecules.

PubMed

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

2009-03-19

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

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

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

Fang, Yu; Zhou, Feng; Yang, Junyi

2015-06-22

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

Photon gating in four-dimensional ultrafast electron microscopy.

PubMed

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

2015-10-20

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

Photon gating in four-dimensional ultrafast electron microscopy

PubMed Central

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

2015-01-01

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

Structure and Dynamics with Ultrafast Electron Microscopes

NASA Astrophysics Data System (ADS)

Siwick, Bradley

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

Ultrafast optical switching of infrared plasmon polaritons in high-mobility graphene

NASA Astrophysics Data System (ADS)

Ni, G. X.; Wang, L.; Goldflam, M. D.; Wagner, M.; Fei, Z.; McLeod, A. S.; Liu, M. K.; Keilmann, F.; Özyilmaz, B.; Castro Neto, A. H.; Hone, J.; Fogler, M. M.; Basov, D. N.

2016-04-01

The success of metal-based plasmonics for manipulating light at the nanoscale has been empowered by imaginative designs and advanced nano-fabrication. However, the fundamental optical and electronic properties of elemental metals, the prevailing plasmonic media, are difficult to alter using external stimuli. This limitation is particularly restrictive in applications that require modification of the plasmonic response at sub-picosecond timescales. This handicap has prompted the search for alternative plasmonic media, with graphene emerging as one of the most capable candidates for infrared wavelengths. Here we visualize and elucidate the properties of non-equilibrium photo-induced plasmons in a high-mobility graphene monolayer. We activate plasmons with femtosecond optical pulses in a specimen of graphene that otherwise lacks infrared plasmonic response at equilibrium. In combination with static nano-imaging results on plasmon propagation, our infrared pump-probe nano-spectroscopy investigation reveals new aspects of carrier relaxation in heterostructures based on high-purity graphene.

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

DOE PAGES

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

2016-08-02

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

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

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

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

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

Quantum and Classical Plasmonic Phenomena in Nanoparticle Arrays

NASA Astrophysics Data System (ADS)

Govorov, Alexander; Besteiro, Lucas; Khosravi Khorashad, Larousse; Kong, Xiang-Tian; Roller, Eva-Maria; Liedl, Tim

Using both classical and quantum approaches, we model plasmonic phenomena in nanoparticle (NP) dimers and trimers. Using a model of three nanoparticles, we propose a mechanism of non-dissipative and ultrafast plasmon passage assisted by hot spots. For this, the NP trimer should include two Au-NPs and one Ag-NP. In the Au-Ag-Au trimer, the two Au-plasmons become coupled via the virtual plasmon of the Ag-NP. The efficient and ultra-fast passage of the Au-plasmons assisted by the virtual Ag-plasmon only becomes possible when the inter-NP gaps in the trimer are small. In this coupling regime, the inter-NP gap regions become plasmonic hot spots that greatly enhance the plasmonic passage effect. At this moment, the plasmonic passage phenomenon was already observed experimentally using optical spectroscopy and the DNA-origami NP complexes. Other systems of our interest were a NP dimer and a nanostar with plasmonic hot spots. For those systems, we predict strong enhancement of the generation of energetic (hot) carriers.

Structural, optical and vibrational properties of self-assembled Pbn+1(Ti1−xFex)nO3n+1−δ Ruddlesden-Popper superstructures

PubMed Central

Doig, K. I.; Peters, J. J. P.; Nawaz, S.; Walker, D.; Walker, M.; Lees, M. R.; Beanland, R.; Sanchez, A. M.; McConville, C. F.; Palkar, V. R.; Lloyd-Hughes, J.

2015-01-01

Bulk crystals and thin films of PbTi1−xFexO3−δ (PTFO) are multiferroic, exhibiting ferroelectricity and ferromagnetism at room temperature. Here we report that the Ruddlesden-Popper phase Pbn+1(Ti1−xFex)nO3n+1−δ forms spontaneously during pulsed laser deposition of PTFO on LaAlO3 substrates. High-resolution transmission electron microscopy, x-ray diffraction and x-ray photoemission spectroscopy were utilised to perform a structural and compositional analysis, demonstrating that and . The complex dielectric function of the films was determined from far-infrared to ultraviolet energies using a combination of terahertz time-domain spectroscopy, Fourier transform spectroscopy, and spectroscopic ellipsometry. The simultaneous Raman and infrared activity of phonon modes and the observation of second harmonic generation establishes a non-centrosymmetric point group for Pbn+1(Ti0.5Fe0.5)nO3n+1−δ, a prerequisite for (but not proof of) ferroelectricity. No evidence of macroscopic ferromagnetism was found in SQUID magnetometry. The ultrafast optical response exhibited coherent magnon oscillations compatible with local magnetic order, and additionally was used to study photocarrier cooling on picosecond timescales. An optical gap smaller than that of BiFeO3 and long photocarrier lifetimes may make this system interesting as a ferroelectric photovoltaic. PMID:25591924

Direct Characterization of Ultrafast Energy-Time Entangled Photon Pairs.

PubMed

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

2018-02-02

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

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

PubMed Central

2015-01-01

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

Optical Manipulation and Detection of Emergent Phenomena in Topological Insulators

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

Gedik, Nuh

The three-dimensional topological insulator (TI) is a new quantum phase of matter that exhibits quantum-Hall-like properties, even in the absence of an external magnetic field. These materials are insulators in the bulk but have a topologically protected conducting state at the surface. Charge carriers on these surface states behave like a two-dimensional gas of massless helical Dirac fermions for which the spin is ideally locked perpendicular to the momentum. The purpose of this project is to probe the unique collective electronic behaviors of topological insulators by developing and using advanced time resolved spectroscopic techniques with state-of-the-art temporal and spatial resolutions.more » The nature of these materials requires development of specialized ultrafast techniques (such as time resolved ARPES that also has spin detection capability, ultrafast electron diffraction that has sub-100 fs time resolution and THz magneto-spectroscopy). The focus of this report is to detail our achievements in terms of establishing state of the art experimental facilities. Below, we will describe achievements under this award for the entire duration of five years. We will focus on detailing the development of ultrafast technqiues here. The details of the science that was done with these technqiues can be found in the publications referencing this grant.« less

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.

Frequency and amplitude modulation of ultra-compact terahertz quantum cascade lasers using an integrated avalanche diode oscillator.

PubMed

Castellano, Fabrizio; Li, Lianhe; Linfield, Edmund H; Davies, A Giles; Vitiello, Miriam S

2016-03-15

Mode-locked comb sources operating at optical frequencies underpin applications ranging from spectroscopy and ultrafast physics, through to absolute frequency measurements and atomic clocks. Extending their operation into the terahertz frequency range would greatly benefit from the availability of compact semiconductor-based sources. However, the development of any compact mode-locked THz laser, which itself is inherently a frequency comb, has yet to be achieved without the use of an external stimulus. High-power, electrically pumped quantum cascade lasers (QCLs) have recently emerged as a promising solution, owing to their octave spanning bandwidths, the ability to achieve group-velocity dispersion compensation and the possibility of obtaining active mode-locking. Here, we propose an unprecedented compact architecture to induce both frequency and amplitude self-modulation in a THz QCL. By engineering a microwave avalanche oscillator into the laser cavity, which provides a 10 GHz self-modulation of the bias current and output power, we demonstrate multimode laser emission centered around 3 THz, with distinct multiple sidebands. The resulting microwave amplitude and frequency self-modulation of THz QCLs opens up intriguing perspectives, for engineering integrated self-mode-locked THz lasers, with impact in fields such as nano- and ultrafast photonics and optical metrology.

Frequency and amplitude modulation of ultra-compact terahertz quantum cascade lasers using an integrated avalanche diode oscillator

PubMed Central

Castellano, Fabrizio; Li, Lianhe; Linfield, Edmund H.; Davies, A. Giles; Vitiello, Miriam S.

2016-01-01

Mode-locked comb sources operating at optical frequencies underpin applications ranging from spectroscopy and ultrafast physics, through to absolute frequency measurements and atomic clocks. Extending their operation into the terahertz frequency range would greatly benefit from the availability of compact semiconductor-based sources. However, the development of any compact mode-locked THz laser, which itself is inherently a frequency comb, has yet to be achieved without the use of an external stimulus. High-power, electrically pumped quantum cascade lasers (QCLs) have recently emerged as a promising solution, owing to their octave spanning bandwidths, the ability to achieve group-velocity dispersion compensation and the possibility of obtaining active mode-locking. Here, we propose an unprecedented compact architecture to induce both frequency and amplitude self-modulation in a THz QCL. By engineering a microwave avalanche oscillator into the laser cavity, which provides a 10 GHz self-modulation of the bias current and output power, we demonstrate multimode laser emission centered around 3 THz, with distinct multiple sidebands. The resulting microwave amplitude and frequency self-modulation of THz QCLs opens up intriguing perspectives, for engineering integrated self-mode-locked THz lasers, with impact in fields such as nano- and ultrafast photonics and optical metrology. PMID:26976199

Watching the dynamics of electrons and atoms at work in solar energy conversion

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

Canton, S. E.; Zhang, X.; Liu, Y.

2015-07-06

The photochemical reactions performed by transition metal complexes have been proposed as viable routes towards solar energy conversion and storage into other forms that can be conveniently used in our everyday applications. In order to develop efficient materials, it is necessary to identify, characterize and optimize the elementary steps of the entire process on the atomic scale. To this end, we have studied the photoinduced electronic and structural dynamics in two heterobimetallic ruthenium–cobalt dyads, which belong to the large family of donor–bridge–acceptor systems. Using a combination of ultrafast optical and X-ray absorption spectroscopies, we can clock the light-driven electron transfermore » processes with element and spin sensitivity. In addition, the changes in local structure around the two metal centers are monitored. These experiments show that the nature of the connecting bridge is decisive for controlling the forward and the backward electron transfer rates, a result supported by quantum chemistry calculations. More generally, this work illustrates how ultrafast optical and X-ray techniques can disentangle the influence of spin, electronic and nuclear factors on the intramolecular electron transfer process. Finally, some implications for further improving the design of bridged sensitizer-catalysts utilizing the presented methodology are outlined.« less

Colloidal thallium halide nanocrystals with reasonable luminescence, carrier mobility and diffusion length† †Electronic supplementary information (ESI) available: Synthesis and additional characterization of nanocrystals, characterization of nanocrystal films, temperature-dependent phase transition, coefficient of volume expansion, PL decay dynamics, tabulated best fit parameters, and methodology analysis of ultrafast optical pump THz probe (OPTP) spectroscopy. See DOI: 10.1039/c7sc01219e Click here for additional data file.

PubMed Central

Mir, Wasim J.; Warankar, Avinash; Acharya, Ashutosh; Das, Shyamashis

2017-01-01

Colloidal lead halide based perovskite nanocrystals (NCs) have been recently established as an interesting class of defect-tolerant NCs with potential for superior optoelectronic applications. The electronic band structure of thallium halides (TlX, where X = Br and I) show a strong resemblance to lead halide perovskites, where both Pb2+ and Tl+ exhibit a 6s2 inert pair of electrons and strong spin–orbit coupling. Although the crystal structure of TlX is not perovskite, the similarities of its electronic structure with lead halide perovskites motivated us to prepare colloidal TlX NCs. These TlX NCs exhibit a wide bandgap (>2.5 eV or <500 nm) and the potential to exhibit a reduced density of deep defect states. Optical pump terahertz (THz) probe spectroscopy with excitation fluence in the range of 0.85–5.86 × 1013 photons per cm2 on NC films shows that the TlBr NCs possess high effective carrier mobility (∼220 to 329 cm2 V–1 s–1), long diffusion length (∼0.77 to 0.98 μm), and reasonably high photoluminescence efficiency (∼10%). This combination of properties is remarkable compared to other wide-bandgap (>2.5 eV) semiconductor NCs, which suggests a reduction in the deep-defect states in the TlX NCs. Furthermore, the ultrafast carrier dynamics and temperature-dependent reversible structural phase transition together with its influence on the optical properties of the TlX NCs are studied. PMID:28970882

Distinctive Spectral Features of Exciton and Excimer States in the Ultrafast Electronic Deactivation of the Adenine Dinucleotide

NASA Astrophysics Data System (ADS)

Stuhldreier, Mayra C.; Röttger, Katharina; Temps, Friedrich

We report the observation by transient absorption spectroscopy of distinctive spectro-temporal signatures of delocalized exciton versus relaxed, weakly bound excimer states in the ultrafast electronic deactivation after UV photoexcitation of the adenine dinucleotide.

Optothermal response of a single silicon nanotip

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

Ultimate waveform reproducibility of extreme-ultraviolet pulses by high-harmonic generation in quartz

NASA Astrophysics Data System (ADS)

Garg, M.; Kim, H. Y.; Goulielmakis, E.

2018-05-01

Optical waveforms of light reproducible with subcycle precision underlie applications of lasers in ultrafast spectroscopies, quantum control of matter and light-based signal processing. Nonlinear upconversion of optical pulses via high-harmonic generation in gas media extends these capabilities to the extreme ultraviolet (EUV). However, the waveform reproducibility of the generated EUV pulses in gases is inherently sensitive to intensity and phase fluctuations of the driving field. We used photoelectron interferometry to study the effects of intensity and carrier-envelope phase of an intense single-cycle optical pulse on the field waveform of EUV pulses generated in quartz nanofilms, and contrasted the results with those obtained in gas argon. The EUV waveforms generated in quartz were found to be virtually immune to the intensity and phase of the driving field, implying a non-recollisional character of the underlying emission mechanism. Waveform-sensitive photonic applications and precision measurements of fundamental processes in optics will benefit from these findings.

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.

Physicochemical characterization and failure analysis of military coating systems

NASA Astrophysics Data System (ADS)

Keene, Lionel Thomas

Modern military coating systems, as fielded by all branches of the U.S. military, generally consist of a diverse array of organic and inorganic components that can complicate their physicochemical analysis. These coating systems consist of VOC-solvent/waterborne automotive grade polyurethane matrix containing a variety of inorganic pigments and flattening agents. The research presented here was designed to overcome the practical difficulties regarding the study of such systems through the combined application of several cross-disciplinary techniques, including vibrational spectroscopy, electron microscopy, microtomy, ultra-fast laser ablation and optical interferometry. The goal of this research has been to determine the degree and spatial progression of weathering-induced alteration of military coating systems as a whole, as well as to determine the failure modes involved, and characterizing the impact of these failures on the physical barrier performance of the coatings. Transmission-mode Fourier Transform Infrared (FTIR) spectroscopy has been applied to cross-sections of both baseline and artificially weathered samples to elucidate weathering-induced spatial gradients to the baseline chemistry of the coatings. A large discrepancy in physical durability (as indicated by the spatial progression of these gradients) has been found between older and newer generation coatings. Data will be shown implicating silica fillers (previously considered inert) as the probable cause for this behavioral divergence. A case study is presented wherein the application of the aforementioned FTIR technique fails to predict the durability of the coating system as a whole. The exploitation of the ultra-fast optical phenomenon of femtosecond (10-15S) laser ablation is studied as a potential tool to facilitate spectroscopic depth profiling of composite materials. Finally, the interferometric technique of Phase Shifting was evaluated as a potential high-sensitivity technique applied to the problem of determining internal stress evolution in curing and aging coatings.

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

PubMed

Kraack, Jan Philip

2017-10-25

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

Graphene-clad microfibre saturable absorber for ultrafast fibre lasers.

PubMed

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

2016-05-16

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

Graphene-clad microfibre saturable absorber for ultrafast fibre lasers

PubMed Central

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

2016-01-01

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

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.

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.

Ultrahigh photoconductivity of bandgap-graded CdSxSe1-x nanowires probed by terahertz spectroscopy

NASA Astrophysics Data System (ADS)

Liu, Hongwei; Lu, Junpeng; Yang, Zongyin; Teng, Jinghua; Ke, Lin; Zhang, Xinhai; Tong, Limin; Sow, Chorng Haur

2016-06-01

Superiorly high photoconductivity is desirable in optoelectronic materials and devices for information transmission and processing. Achieving high photoconductivity via bandgap engineering in a bandgap-graded semiconductor nanowire has been proposed as a potential strategy. In this work, we report the ultrahigh photoconductivity of bandgap-graded CdSxSe1-x nanowires and its detailed analysis by means of ultrafast optical-pump terahertz-probe (OPTP) spectroscopy. The recombination rates and carrier mobility are quantitatively obtained via investigation of the transient carrier dynamics in the nanowires. By analysis of the terahertz (THz) spectra, we obtain an insight into the bandgap gradient and band alignment to carrier transport along the nanowires. The demonstration of the ultrahigh photoconductivity makes bandgap-graded CdSxSe1-x nanowires a promising candidate as building blocks for nanoscale electronic and photonic devices.

Coherent Multidimensional Core Spectroscopy of Molecules with Multiple X-ray pulses

NASA Astrophysics Data System (ADS)

Mukamel, Shaul

2017-04-01

Multidimensional spectroscopy uses sequences of optical pulses to study dynamical processes in complex molecules through correlation plots involving several time delay periods. Extensions of these techniques to the x-ray regime will be discussed. Ultrafast nonlinear x-ray spectroscopy is made possible by newly developed free electron laser and high harmonic generation sources. The attosecond duration of X-ray pulses and the atomic selectivity of core X-ray excitations offer a uniquely high spatial and temporal resolution. We demonstrate how stimulated Raman detection of an X-ray probe may be used to monitor the phase and dynamics of the nonequilibrium valence electronic state wavepacket created by e.g. photoexcitation, photoionization and Auger processes. Spectroscopy of multiplecore excitations provides a new window into electron correlations. Applications will be presented to long-range charge transfer in proteins and to excitation energy transfer in porphyrin arrays. Conical intersections (CoIn) dominate the pathways and outcomes of virtually all photophysical and photochemical molecular processes. Despite extensive experimental and theoretical effort CoIns have not been directly observed yet and the experimental evidence is being inferred from fast reaction rates and some vibrational signatures. Novel ultrafast X ray probes for these processes will be presented. Short X-ray pulses can directly detect the passage through a CoIn with the adequate temporal and spectral sensitivity. The technique is based on a coherent Raman process that employs a composite femtosecond/attosecond X-ray pulse to directly detect the electronic coherences (rather than populations) that are generated as the system passes through the CoIn. Streaking of time-resolved photoelectron spectroscopy (TRPES) signals offers another powerful window into the joint electronic/vibrational dynamics at concial intersections. Strong coupling of molecules to the vacuum field of micro cavities can modify the potential energy surfaces thereby manipulating the photophysical and photochemical reaction pathways. The photonic vacuum state of a localized cavity mode can be strongly mixed with the molecular degrees of freedom to create hybrid field-matter states known as polaritons. Simulations of the avoided crossing of sodium iodide in a cavity which incorporate the quantized cavity field into the nuclear wave packet dynamics will be presented. Numerical results show how the branching ratio between the covalent and ionic dissociation channels can be strongly manipulated by the optical cavity.

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

PubMed

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

2017-08-03

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

Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom

NASA Astrophysics Data System (ADS)

Brauße, Felix; Goldsztejn, Gildas; Amini, Kasra; Boll, Rebecca; Bari, Sadia; Bomme, Cédric; Brouard, Mark; Burt, Michael; de Miranda, Barbara Cunha; Düsterer, Stefan; Erk, Benjamin; Géléoc, Marie; Geneaux, Romain; Gentleman, Alexander S.; Guillemin, Renaud; Ismail, Iyas; Johnsson, Per; Journel, Loïc; Kierspel, Thomas; Köckert, Hansjochen; Küpper, Jochen; Lablanquie, Pascal; Lahl, Jan; Lee, Jason W. L.; Mackenzie, Stuart R.; Maclot, Sylvain; Manschwetus, Bastian; Mereshchenko, Andrey S.; Mullins, Terence; Olshin, Pavel K.; Palaudoux, Jérôme; Patchkovskii, Serguei; Penent, Francis; Piancastelli, Maria Novella; Rompotis, Dimitrios; Ruchon, Thierry; Rudenko, Artem; Savelyev, Evgeny; Schirmel, Nora; Techert, Simone; Travnikova, Oksana; Trippel, Sebastian; Underwood, Jonathan G.; Vallance, Claire; Wiese, Joss; Simon, Marc; Holland, David M. P.; Marchenko, Tatiana; Rouzée, Arnaud; Rolles, Daniel

2018-04-01

Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I ) is investigated by ionization above the iodine 4 d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

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

NASA Astrophysics Data System (ADS)

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

2016-05-01

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

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

PubMed

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

2018-05-24

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

Two-Dimensional CH3NH3PbI3 Perovskite Nanosheets for Ultrafast Pulsed Fiber Lasers.

PubMed

Li, Pengfei; Chen, Yao; Yang, Tieshan; Wang, Ziyu; Lin, Han; Xu, Yanhua; Li, Lei; Mu, Haoran; Shivananju, Bannur Nanjunda; Zhang, Yupeng; Zhang, Qinglin; Pan, Anlian; Li, Shaojuan; Tang, Dingyuan; Jia, Baohua; Zhang, Han; Bao, Qiaoliang

2017-04-12

Even though the nonlinear optical effects of solution processed organic-inorganic perovskite films have been studied, the nonlinear optical properties in two-dimensional (2D) perovskites, especially their applications for ultrafast photonics, are largely unexplored. In comparison to bulk perovskite films, 2D perovskite nanosheets with small thicknesses of a few unit cells are more suitable for investigating the intrinsic nonlinear optical properties because bulk recombination of photocarriers and the nonlinear scattering are relatively small. In this research, we systematically investigated the nonlinear optical properties of 2D perovskite nanosheets derived from a combined solution process and vapor phase conversion method. It was found that 2D perovskite nanosheets have stronger saturable absorption properties with large modulation depth and very low saturation intensity compared with those of bulk perovskite films. Using an all dry transfer method, we constructed a new type of saturable absorber device based on single piece 2D perovskite nanosheet. Stable soliton state mode-locking was achieved, and ultrafast picosecond pulses were generated at 1064 nm. This work is likely to pave the way for ultrafast photonic and optoelectronic applications based on 2D perovskites.

Novel optoelectronic devices; Proceedings of the Meeting, The Hague, Netherlands, Mar. 31-Apr. 2, 1987

NASA Technical Reports Server (NTRS)

Adams, Michael J. (Editor)

1987-01-01

The present conference on novel optoelectronics discusses topics in the state-of-the-art in this field in the Netherlands, quantum wells, integrated optics, nonlinear optical devices and fiber-optic-based devices, ultrafast optics, and nonlinear optics and optical bistability. Attention is given to the production of fiber-optics for telecommunications by means of PCVD, lifetime broadening in quantum wells, nonlinear multiple quantum well waveguide devices, tunable single-wavelength lasers, an Si integrated waveguiding polarimeter, and an electrooptic light modulator using long-range surface plasmons. Also discussed are backward-wave couplers and reflectors, a wavelength-selective all-fiber switching matrix, the impact of ultrafast optics in high-speed electronics, the physics of low energy optical switching, and all-optical logical elements for optical processing.

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

Deb, Marwan, E-mail: marwan.deb@ipcms.unistra.fr; Vomir, Mircea; Rehspringer, Jean-Luc

Controlling the magnetization dynamics on the femtosecond timescale is of fundamental importance for integrated opto-spintronic devices. For industrial perspectives, it requires to develop simple growth techniques for obtaining large area magneto-optical materials having a high amplitude ultrafast Faraday or Kerr response. Here we report on optical pump probe studies of light induced spin dynamics in high quality bismuth doped iron garnet polycrystalline film prepared by the spin coating method. We demonstrate an ultrafast non-thermal optical control of the spin dynamics using both circularly and linearly polarized pulses.

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.

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.

Noncollinear wave mixing of attosecond XUV and few-cycle optical laser pulses in gas-phase atoms: Toward multidimensional spectroscopy involving XUV excitations

NASA Astrophysics Data System (ADS)

Cao, Wei; Warrick, Erika R.; Fidler, Ashley; Neumark, Daniel M.; Leone, Stephen R.

2016-11-01

Ultrafast nonlinear spectroscopy, which records transient wave-mixing signals in a medium, is a powerful tool to access microscopic information using light sources in the radio-frequency and optical regimes. The extension of this technique towards the extreme ultraviolet (XUV) or even x-ray regimes holds the promise to uncover rich structural or dynamical information with even higher spatial or temporal resolution. Here, we demonstrate noncollinear wave mixing between weak XUV attosecond pulses and a strong near-infrared (NIR) few-cycle laser pulse in gas phase atoms (one photon of XUV and two photons of NIR). In the noncollinear geometry the attosecond and either one or two NIR pulses interact with argon atoms. Nonlinear XUV signals are generated in a spatially resolved fashion as required by phase matching. Different transition pathways can be identified from these background-free nonlinear signals according to the specific phase-matching conditions. Time-resolved measurements of the spatially gated XUV signals reveal electronic coherences of Rydberg wave packets prepared by a single XUV photon or XUV-NIR two-photon excitation, depending on the applied pulse sequences. These measurements open possible applications of tabletop multidimensional spectroscopy to the study of dynamics associated with valence or core excitation with XUV photons.

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

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

Advanced optic fabrication using ultrafast laser radiation

NASA Astrophysics Data System (ADS)

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

2016-03-01

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

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

PubMed

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

2016-08-08

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

Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons

PubMed Central

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

2016-01-01

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

Strong negative terahertz photoconductivity in photoexcited graphene

NASA Astrophysics Data System (ADS)

Fu, Maixia; Wang, Xinke; Ye, Jiasheng; Feng, Shengfei; Sun, Wenfeng; Han, Peng; Zhang, Yan

2018-01-01

Terahertz (THz) response of a chemical vapor deposited graphene on a quartz substrate has been investigated by using an ultrafast optical-pump THz-probe spectroscopy. Without photoexcitation, the frequency-dependence optical conductivity shows a strong carrier response owing to the intrinsically doped graphene. Upon photoexcitation, an enhancement in THz transmission is observed and the transmission increases nonlinearly with the increase of pump power, which is rooted in a reduction of intrinsic conductivity arising from the strong enhancement of carrier scattering rather than THz emission occurrence. The modulation depth of 18.8% was experimentally achieved, which is more than four times greater than that of the previous reported. The photoinduced response here highlights the variety of response possible in graphene depending on the sample quality, carrier mobility and doping level. The graphene provides promising applications in high-performance THz modulators and THz photoelectric devices.

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

NASA Astrophysics Data System (ADS)

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

2017-11-01

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

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

PubMed Central

2014-01-01

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

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

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

NASA Technical Reports Server (NTRS)

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

2005-01-01

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

Ultrafast Graphene Light Emitters.

PubMed

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

2018-02-14

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

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

NASA Astrophysics Data System (ADS)

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

2016-06-01

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

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.

Mapping momentum-dependent electron-phonon coupling and nonequilibrium phonon dynamics with ultrafast electron diffuse scattering

NASA Astrophysics Data System (ADS)

Stern, Mark J.; René de Cotret, Laurent P.; Otto, Martin R.; Chatelain, Robert P.; Boisvert, Jean-Philippe; Sutton, Mark; Siwick, Bradley J.

2018-04-01

Despite their fundamental role in determining material properties, detailed momentum-dependent information on the strength of electron-phonon and phonon-phonon coupling (EPC and PPC, respectively) across the entire Brillouin zone has remained elusive. Here we demonstrate that ultrafast electron diffuse scattering (UEDS) directly provides such information. By exploiting symmetry-based selection rules and time resolution, scattering from different phonon branches can be distinguished even without energy resolution. Using graphite as a model system, we show that UEDS patterns map the relative EPC and PPC strength through their profound sensitivity to photoinduced changes in phonon populations. We measure strong EPC to the K -point TO phonon of A1' symmetry (K -A1' ) and along the entire TO branch between Γ -K , not only to the Γ -E2 g phonon. We also determine that the subsequent phonon relaxation of these strongly coupled optical phonons involve three stages: decay via several identifiable channels to TA and LA phonons (1 -2 ps), intraband thermalization of the non-equilibrium TA/LA phonon populations (30 -40 ps) and interband relaxation of the TA/LA modes (115 ps). Combining UEDS with ultrafast angle-resolved photoelectron spectroscopy will yield a complete picture of the dynamics within and between electron and phonon subsystems, helping to unravel complex phases in which the intertwined nature of these systems has a strong influence on emergent properties.

A Dual-Colour Architecture for Pump-Probe Spectroscopy of Ultrafast Magnetization Dynamics in the Sub-10-femtosecond Range.

PubMed

Gonçalves, C S; Silva, A S; Navas, D; Miranda, M; Silva, F; Crespo, H; Schmool, D S

2016-03-15

Current time-resolution-limited dynamic measurements clearly show the need for improved techniques to access processes on the sub-10-femtosecond timescale. To access this regime, we have designed and constructed a state-of-the-art time-resolved magneto-optic Kerr effect apparatus, based on a new dual-color scheme, for the measurement of ultrafast demagnetization and precessional dynamics in magnetic materials. This system can operate well below the current temporal ranges reported in the literature, which typically lie in the region of around 50 fs and above. We have used a dual-colour scheme, based on ultra broadband hollow-core fibre and chirped mirror pulse compression techniques, to obtain unprecedented sub-8-fs pump and probe pulse durations at the sample plane. To demonstrate the capabilities of this system for ultrafast demagnetization and precessional dynamics studies, we have performed measurements in a ferrimagnetic GdFeCo thin film. Our study has shown that the magnetization shows a sudden drop within the first picosecond after the pump pulse, a fast recovery (remagnetization) within a few picoseconds, followed by a clear oscillation or precession during a slower magnetization recovery. Moreover, we have experimentally confirmed for the first time that a sub-10-fs pulse is able to efficiently excite a magnetic system such as GdFeCo.

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

Revealing Extremely Low Energy Amplitude Modes in the Charge-Density-Wave Compound LaAgSb_{2}.

PubMed

Chen, R Y; Zhang, S J; Zhang, M Y; Dong, T; Wang, N L

2017-03-10

Using infrared spectroscopy and ultrafast pump probe measurement, we have studied the two charge-density-wave (CDW) instabilities in the layered compound LaAgSb_{2}. The development of CDW energy gaps was clearly observed by optical spectroscopy, which removed most of the free carrier spectral weight. More interestingly, our time-resolved measurements revealed two coherent oscillations that softened by approaching the two phase transition temperatures, respectively. We addressed that these two oscillations come from the amplitude modes of CDW collective excitations, the surprisingly low energies (0.12 THz and 0.34 THz for the higher and lower temperature ones, respectively) of which are associated with the extremely small nesting wave vectors. Additionally, the amplitude and relaxation time of photoinduced reflectivity of LaAgSb_{2} single crystals stayed unchanged across the CDW phase transitions, which is quite rare and deserves further investigation.

Quantifying highly efficient incoherent energy transfer in perylene-based multichromophore arrays.

PubMed

Webb, James E A; Chen, Kai; Prasad, Shyamal K K; Wojciechowski, Jonathan P; Falber, Alexander; Thordarson, Pall; Hodgkiss, Justin M

2016-01-21

Multichromophore perylene arrays were designed and synthesized to have extremely efficient resonance energy transfer. Using broadband ultrafast photoluminescence and transient absorption spectroscopies, transfer timescales of approximately 1 picosecond were resolved, corresponding to efficiencies of up to 99.98%. The broadband measurements also revealed spectra corresponding to incoherent transfer between localized states. Polarization resolved spectroscopy was used to measure the dipolar angles between donor and acceptor chromophores, thereby enabling geometric factors to be fixed when assessing the validity of Förster theory in this regime. Förster theory was found to predict the correct magnitude of transfer rates, with measured ∼2-fold deviations consistent with the breakdown of the point-dipole approximation at close approach. The materials presented, along with the novel methods for quantifying ultrahigh energy transfer efficiencies, will be valuable for applications demanding extremely efficient energy transfer, including fluorescent solar concentrators, optical gain, and photonic logic devices.

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.

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

PubMed

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

2014-10-28

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

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.

Photoinduced Electron Transfer in the Strong Coupling Regime: Waveguide-Plasmon Polaritons.

PubMed

Zeng, Peng; Cadusch, Jasper; Chakraborty, Debadi; Smith, Trevor A; Roberts, Ann; Sader, John E; Davis, Timothy J; Gómez, Daniel E

2016-04-13

Reversible exchange of photons between a material and an optical cavity can lead to the formation of hybrid light-matter states where material properties such as the work function [ Hutchison et al. Adv. Mater. 2013 , 25 , 2481 - 2485 ], chemical reactivity [ Hutchison et al. Angew. Chem., Int. Ed. 2012 , 51 , 1592 - 1596 ], ultrafast energy relaxation [ Salomon et al. Angew. Chem., Int. Ed. 2009 , 48 , 8748 - 8751 ; Gomez et al. J. Phys. Chem. B 2013 , 117 , 4340 - 4346 ], and electrical conductivity [ Orgiu et al. Nat. Mater. 2015 , 14 , 1123 - 1129 ] of matter differ significantly to those of the same material in the absence of strong interactions with the electromagnetic fields. Here we show that strong light-matter coupling between confined photons on a semiconductor waveguide and localized plasmon resonances on metal nanowires modifies the efficiency of the photoinduced charge-transfer rate of plasmonic derived (hot) electrons into accepting states in the semiconductor material. Ultrafast spectroscopy measurements reveal a strong correlation between the amplitude of the transient signals, attributed to electrons residing in the semiconductor and the hybridization of waveguide and plasmon excitations.

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.

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

NASA Astrophysics Data System (ADS)

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

2015-09-01

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

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.

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.

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

NASA Astrophysics Data System (ADS)

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

2017-11-01

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

Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots

DOE PAGES

Gao, Jianbo; Fidler, Andrew F.; Klimov, Victor I.

2015-09-08

In carrier multiplication, the absorption of a single photon results in two or more electron–hole pairs. Quantum dots are promising materials for implementing carrier multiplication principles in real-life technologies. So far, however, most of research in this area has focused on optical studies of solution samples with yet to be proven relevance to practical devices. We report ultra-fast electro-optical studies of device-grade films of electronically coupled quantum dots that allow us to observe multiplication directly in the photocurrent. Our studies help rationalize previous results from both optical spectroscopy and steady-state photocurrent measurements and also provide new insights into effects ofmore » electric field and ligand treatments on multiexciton yields. Importantly, we demonstrate that using appropriate chemical treatments of the films, extra charges produced by carrier multiplication can be extracted from the quantum dots before they are lost to Auger recombination and hence can contribute to photocurrent of practical devices.« less

Attosecond optical-field-enhanced carrier injection into the GaAs conduction band

NASA Astrophysics Data System (ADS)

Schlaepfer, F.; Lucchini, M.; Sato, S. A.; Volkov, M.; Kasmi, L.; Hartmann, N.; Rubio, A.; Gallmann, L.; Keller, U.

2018-06-01

Resolving the fundamental carrier dynamics induced in solids by strong electric fields is essential for future applications, ranging from nanoscale transistors1,2 to high-speed electro-optical switches3. How fast and at what rate can electrons be injected into the conduction band of a solid? Here, we investigate the sub-femtosecond response of GaAs induced by resonant intense near-infrared laser pulses using attosecond transient absorption spectroscopy. In particular, we unravel the distinct role of intra- versus interband transitions. Surprisingly, we found that despite the resonant driving laser, the optical response during the light-matter interaction is dominated by intraband motion. Furthermore, we observed that the coupling between the two mechanisms results in a significant enhancement of the carrier injection from the valence into the conduction band. This is especially unexpected as the intraband mechanism itself can accelerate carriers only within the same band. This physical phenomenon could be used to control ultrafast carrier excitation and boost injection rates in electronic switches in the petahertz regime.

Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots

PubMed Central

Gao, Jianbo; Fidler, Andrew F.; Klimov, Victor I.

2015-01-01

In carrier multiplication, the absorption of a single photon results in two or more electron–hole pairs. Quantum dots are promising materials for implementing carrier multiplication principles in real-life technologies. So far, however, most of research in this area has focused on optical studies of solution samples with yet to be proven relevance to practical devices. Here we report ultrafast electro-optical studies of device-grade films of electronically coupled quantum dots that allow us to observe multiplication directly in the photocurrent. Our studies help rationalize previous results from both optical spectroscopy and steady-state photocurrent measurements and also provide new insights into effects of electric field and ligand treatments on multiexciton yields. Importantly, we demonstrate that using appropriate chemical treatments of the films, extra charges produced by carrier multiplication can be extracted from the quantum dots before they are lost to Auger recombination and hence can contribute to photocurrent of practical devices. PMID:26345390

Broadband photocarrier dynamics and nonlinear absorption of PLD-grown WTe2 semimetal films

NASA Astrophysics Data System (ADS)

Gao, Wenbin; Huang, Lei; Xu, Jinlong; Chen, Yequan; Zhu, Chunhui; Nie, Zhonghui; Li, Yao; Wang, Xuefeng; Xie, Zhenda; Zhu, Shining; Xu, Jun; Wan, Xiangang; Zhang, Chao; Xu, Yongbing; Shi, Yi; Wang, Fengqiu

2018-04-01

WTe2 is a unique material in the family of transition metal dichalcogenides and it has been proposed as a candidate for type-II Weyl semimetals. However, thus far, studies on the optical properties of this emerging material have been significantly hindered by the lack of large-area, high-quality WTe2 materials. Here, we grow a centimeter-scale, highly crystalline WTe2 ultrathin film (˜35 nm) by a pulsed laser deposition technique. Broadband pump-probe spectroscopy (1.2-2.5 μm) reveals a peculiar ultrafast optical response where an initial photo-bleaching signal (lasting ˜3 ps) is followed by a long-lived photoinduced absorption signature. Nonlinear absorption characterization using femtosecond pulses confirms the saturable absorption response of the WTe2 ultrathin films, and we further demonstrated a mode-locked Thulium fiber laser using a WTe2 absorber. Our work provides important insights into linear and nonlinear optical responses of WTe2 thin films.

Many-body effects in nonlinear optical responses of 2D layered semiconductors

DOE PAGES

Aivazian, Grant; Yu, Hongyi; Wu, Sanfeng; ...

2017-01-05

We performed ultrafast degenerate pump-probe spectroscopy on monolayer WSe2 near its exciton resonance. The observed differential reflectance signals exhibit signatures of strong many-body interactions including the exciton-exciton interaction and free carrier induced band gap renormalization. The exciton-exciton interaction results in a resonance blue shift which lasts for the exciton lifetime (several ps), while the band gap renormalization manifests as a resonance red shift with several tens ps lifetime. Our model based on the many-body interactions for the nonlinear optical susceptibility ts well the experimental observations. The power dependence of the spectra shows that with the increase of pump power, themore » exciton population increases linearly and then saturates, while the free carrier density increases superlinearly, implying that exciton Auger recombination could be the origin of these free carriers. Our model demonstrates a simple but efficient method for quantitatively analyzing the spectra, and indicates the important role of Coulomb interactions in nonlinear optical responses of such 2D materials.« less

Many-body effects in nonlinear optical responses of 2D layered semiconductors

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

Aivazian, Grant; Yu, Hongyi; Wu, Sanfeng

We performed ultrafast degenerate pump-probe spectroscopy on monolayer WSe2 near its exciton resonance. The observed differential reflectance signals exhibit signatures of strong many-body interactions including the exciton-exciton interaction and free carrier induced band gap renormalization. The exciton-exciton interaction results in a resonance blue shift which lasts for the exciton lifetime (several ps), while the band gap renormalization manifests as a resonance red shift with several tens ps lifetime. Our model based on the many-body interactions for the nonlinear optical susceptibility ts well the experimental observations. The power dependence of the spectra shows that with the increase of pump power, themore » exciton population increases linearly and then saturates, while the free carrier density increases superlinearly, implying that exciton Auger recombination could be the origin of these free carriers. Our model demonstrates a simple but efficient method for quantitatively analyzing the spectra, and indicates the important role of Coulomb interactions in nonlinear optical responses of such 2D materials.« less

Long-period fiber gratings as ultrafast optical differentiators.

PubMed

Kulishov, Mykola; Azaña, José

2005-10-15

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

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

NASA Astrophysics Data System (ADS)

Nurmohammadi, Tofiq; Abbasian, Karim; Yadipour, Reza

2018-03-01

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

Ultrafast all-optical technologies for bidirectional optical wireless communications.

PubMed

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

2015-04-01

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

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

NASA Astrophysics Data System (ADS)

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

2014-04-01

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

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

PubMed Central

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

2014-01-01

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

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

PubMed

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

2017-03-03

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

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

DOE PAGES

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

2014-04-17

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

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

NASA Astrophysics Data System (ADS)

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

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

Ultrafast optical ranging using microresonator soliton frequency combs

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

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

PubMed Central

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

2017-01-01

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

Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons

DOE PAGES

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

2016-03-17

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

Ultrafast third-order nonlinear optical response of pyrene derivatives

NASA Astrophysics Data System (ADS)

Shi, Yufang; Li, Zhongguo; Fang, Yu; Sun, Jinyu; Zhao, Minggen; Song, Yinglin

2017-05-01

Two mono-substituted pyrene derivatives with delocalized electron system 1-(pyren-1-yl)-3-(4-Methyl thiophene-2-yl) acrylic ketone (13#) and 1-(pyren-1-yl)-3-(4-bromo thiophene-2-yl) acrylic ketone (15#) were successfully synthesized. The resultant compounds were characterized by nuclear magnetic resonance (NMR), infrared spectroscopy (IR), high resolution mass spectrum (HR-MS), and UV-vis spectra. The third-order nonlinear optical properties of the compounds were investigated using Z-scan technique with femtosecond laser pulses at 500 nm and 700 nm, respectively. Both of the compounds showed a decrease in transmittance about the focus, which are typical of two-photon absorption. It was found that the two-photon absorption behavior of the pyrene derivatives were modified by substituents on thiophene ring. These results indicate that both compounds can be promising candidates for future optoelectronic and bio-imaging applications.

Evidence for impact ionization in vanadium dioxide

DOE PAGES

Holleman, Joshua; Bishop, Michael M.; Garcia, Carlos; ...

2016-10-17

Pump-probe optical spectroscopy was used to investigate charge carrier multiplication via impact ionization in the M 1 insulating phase of VO 2. By comparing the transient reflectivities of the film when pumped at less than and then more than twice the band-gap energy, we observed an enhancement of the ultrafast response with the higher energy pump color while the film was still transiently in the insulating phase. We additionally identified multiple timescales within the charge dynamics and analyzed how these changed when the pump and probe wavelengths were varied. This experiment provided evidence that impact ionization acts efficiently as amore » carrier multiplication process in this prototypical strongly-correlated insulator.« less

Measuring phonon mean free path distributions by probing quasiballistic phonon transport in grating nanostructures

DOE PAGES

Zeng, Lingping; Collins, Kimberlee C.; Hu, Yongjie; ...

2015-11-27

Heat conduction in semiconductors and dielectrics depends upon their phonon mean free paths that describe the average travelling distance between two consecutive phonon scattering events. Nondiffusive phonon transport is being exploited to extract phonon mean free path distributions. Here, we describe an implementation of a nanoscale thermal conductivity spectroscopy technique that allows for the study of mean free path distributions in optically absorbing materials with relatively simple fabrication and a straightforward analysis scheme. We pattern 1D metallic grating of various line widths but fixed gap size on sample surfaces. The metal lines serve as both heaters and thermometers in time-domainmore » thermoreflectance measurements and simultaneously act as wiregrid polarizers that protect the underlying substrate from direct optical excitation and heating. We demonstrate the viability of this technique by studying length-dependent thermal conductivities of silicon at various temperatures. The thermal conductivities measured with different metal line widths are analyzed using suppression functions calculated from the Boltzmann transport equation to extract the phonon mean free path distributions with no calibration required. Furthermore, this table-top ultrafast thermal transport spectroscopy technique enables the study of mean free path spectra in a wide range of technologically important materials.« less

Modeling Photochemical Dynamics in Optically Active Energetic Materials

NASA Astrophysics Data System (ADS)

Nelson, Tammie; Bjorgaard, Josiah; Greenfield, Margo; Bolme, Cindy; Brown, Katie; McGrane, Shawn; Scharff, R. Jason; Tretiak, Sergei

Most high explosives (HEs) absorb in the UV range, making it difficult to develop HEs that can be excited with standard lasers. The conventional optical initiation mechanisms require high laser intensity and occur via indirect thermal or shock processes. A photochemical initiation mechanism could allow control over the chemistry contributing to decomposition leading to initiation. We combine UV femtosecond transient absorption (TA) spectroscopy and excited state femtosecond stimulated Raman spectroscopy (FSRS) with Nonadiabatic Excited State Molecular Dynamics (NA-ESMD) to model the photochemical pathways in nitromethane (NM), a low sensitivity HE known to undergo UV photolysis. We investigate the ultrafast photodecomposition of NM from the nπ* state excited at 266 nm. The FSRS photoproduct spectrum points to methyl nitrite formation as the dominant photoproduct. A total photolysis quantum yield of 0.27 and an nπ* state lifetime of 20 fs were predicted from simulations. Predicted time scales reveal that NO2 dissociation occurs in 81 +/-4 fs and methyl nitrite formation is much slower at 452 +/-9 fs corresponding to the absorption feature in the TA spectrum. The relative time scales are consistent with isomerization by NO2 dissociation and ONO rebinding.

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

PubMed

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

2014-07-25

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

Ultrafast studies of organometallic photochemistry: The mechanism of carbon-hydrogen bond activation in solution

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

Bromberg, S.E.

1998-05-01

When certain organometallic compounds are photoexcited in room temperature alkane solution, they are able to break or activate the C-H bonds of the solvent. Understanding this potentially practical reaction requires a detailed knowledge of the entire reaction mechanism. Because of the dynamic nature of chemical reactions, time-resolved spectroscopy is commonly employed to follow the important events that take place as reactants are converted to products. For the organometallic reactions examined here, the electronic/structural characteristics of the chemical systems along with the time scales for the key steps in the reaction make ultrafast UV/Vis and IR spectroscopy along with nanosecond Step-Scanmore » FTIR spectroscopy the ideal techniques to use for this study. An initial study of the photophysics of (non-activating) model metal carbonyls centering on the photodissociation of M(CO){sub 6} (M = Cr, W, Mo) was carried out in alkane solutions using ultrafast IR spectroscopy. Next, picosecond UV/vis studies of the C-H bond activation reaction of Cp{sup *}M(CO){sub 2} (M = Rh, Ir), conducted in room temperature alkane solution, are described in an effort to investigate the origin of the low quantum yield for bond cleavage ({approximately}1%). To monitor the chemistry that takes place in the reaction after CO is lost, a system with higher quantum yield is required. The reaction of Tp{sup *}Rh(CO){sub 2} (Tp{sup *} = HB-Pz{sub 3}{sup *}, Pz{sup *} = 3,5-dimethylpyrazolyl) in alkanes has a quantum yield of {approximately}30%, making time resolved spectroscopic measurements possible. From ultrafast IR experiments, two subsequently formed intermediates were observed. The nature of these intermediates are discussed and the first comprehensive reaction mechanism for a photochemical C-H activating organometallic complex is presented.« less

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

PubMed

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

2018-04-24

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

Ultrafast transient grating radiation to optical image converter

DOEpatents

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

2014-11-04

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

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

PubMed

Serebryannikov, E E; Zheltikov, A M

2014-07-25

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

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

PubMed

Hutchings, D C

1995-08-01

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

Ultrafast Graphene Photonics and Optoelectronics

DTIC Science & Technology

2017-04-14

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

Enhanced Ultrafast Nonlinear Optics With Microstructure Fibers And Photonic Crystals

DTIC Science & Technology

2004-07-01

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

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.

Shaping ultrafast laser inscribed optical waveguides using a deformable mirror.

PubMed

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

2008-08-18

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

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.

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.

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

PubMed

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

2017-01-11

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

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

DOEpatents

Heebner, John E [Livermore, CA

2010-08-03

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

Ultrafast optical excitations in supramolecular metallacycles with charge transfer properties.

PubMed

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

2010-02-03

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

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

PubMed

Fushitani, Mizuho; Hishikawa, Akiyoshi

2016-11-01

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

Ultrafast core-loss spectroscopy in four-dimensional electron microscopy

PubMed Central

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

2015-01-01

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

Spin-controlled ultrafast vertical-cavity surface-emitting lasers

NASA Astrophysics Data System (ADS)

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

2014-05-01

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

Optical detection of three modes of endocytosis at hippocampal synapses

PubMed Central

Chanaday, Natali L

2018-01-01

Coupling of synaptic vesicle fusion and retrieval constitutes a core mechanism ensuring maintenance of presynaptic function. Recent studies using fast-freeze electron microscopy and capacitance measurements reported an ultrafast mode of endocytosis operating at physiological temperatures. Here, using rat hippocampal neurons, we optically monitored single synaptic vesicle endocytosis with high time resolution using the vesicular glutamate transporter, synaptophysin and the V0a1 subunit of the vacuolar ATPase as probes. In this setting, we could distinguish three components of retrieval operating at ultrafast (~150–250 ms, ~20% of events), fast (~5–12 s, ~40% of events) and ultraslow speeds (>20 s, ~40% of events). While increasing Ca2+ slowed the fast events, increasing temperature accelerated their time course. In contrast, the kinetics of ultrafast events were only mildly affected by these manipulations. These results suggest that synaptic vesicle proteins can be retrieved with ultrafast kinetics, although a majority of evoked fusion events are coupled to slower retrieval mechanisms. PMID:29683423

Harmonium: An Ultrafast Vacuum Ultraviolet Facility.

PubMed

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

2017-05-31

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

Ultrafast 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.

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

NASA Astrophysics Data System (ADS)

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

2016-10-01

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

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

PubMed Central

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

2016-01-01

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

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

PubMed

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

2016-10-20

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

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

PubMed

Liu, Xiaofeng; Guo, Qiangbing; Qiu, Jianrong

2017-04-01

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

Critical behavior within 20 fs drives the out-of-equilibrium laser-induced magnetic phase transition in nickel

PubMed Central

Tengdin, Phoebe; You, Wenjing; Chen, Cong; Shi, Xun; Zusin, Dmitriy; Zhang, Yingchao; Gentry, Christian; Blonsky, Adam; Keller, Mark; Oppeneer, Peter M.; Kapteyn, Henry C.; Tao, Zhensheng; Murnane, Margaret M.

2018-01-01

It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date, the connection between out-of-equilibrium and equilibrium phase transitions, or how fast the out-of-equilibrium phase transitions can proceed, was not known. By combining time- and angle-resolved photoemission with time-resolved transverse magneto-optical Kerr spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: The spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, whereas demagnetization and the collapse of the exchange splitting occur on much longer, fluence-independent time scales of ~176 fs. Third, we find that the transient electron temperature alone dictates the magnetic response. Our results are important because they connect the out-of-equilibrium material behavior to the strongly coupled equilibrium behavior and uncover a new time scale in the process of ultrafast demagnetization. PMID:29511738

Critical behavior within 20 fs drives the out-of-equilibrium laser-induced magnetic phase transition in nickel.

PubMed

Tengdin, Phoebe; You, Wenjing; Chen, Cong; Shi, Xun; Zusin, Dmitriy; Zhang, Yingchao; Gentry, Christian; Blonsky, Adam; Keller, Mark; Oppeneer, Peter M; Kapteyn, Henry C; Tao, Zhensheng; Murnane, Margaret M

2018-03-01

It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date, the connection between out-of-equilibrium and equilibrium phase transitions, or how fast the out-of-equilibrium phase transitions can proceed, was not known. By combining time- and angle-resolved photoemission with time-resolved transverse magneto-optical Kerr spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: The spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, whereas demagnetization and the collapse of the exchange splitting occur on much longer, fluence-independent time scales of ~176 fs. Third, we find that the transient electron temperature alone dictates the magnetic response. Our results are important because they connect the out-of-equilibrium material behavior to the strongly coupled equilibrium behavior and uncover a new time scale in the process of ultrafast demagnetization.

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.

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

NASA Astrophysics Data System (ADS)

Kim, Jungho

2013-10-01

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

Optoelectronic properties of type I indium gallium arsenide quantum cascade lasers with applications to optical modulation

NASA Astrophysics Data System (ADS)

Murawski, Robert K.

Quantum Cascade Lasers (QCL) are unique unipolar conduction band devices designed to emit in the mid infrared region (MIR). They have been employed very successfully in spectroscopy and sensing applications. Motivated by predictions of modulation bandwidths above 100 GHz, communication links based on QCLs were recently demonstrated. However, the intrinsic device circuitry of the QCL limits its bandwidth. In this thesis a new All-Optical Modulation of the QCL is presented and investigated both theoretically and experimentally. This method of modulation allows for full access to the bandwidth as well as unique optical control of the MIR laser emission. For this purpose, conduction and valence band wave functions for the complex QCL structure are presented allowing for the first time calculations of their interband energy resonances. Based on this knowledge, a novel optical modulation scheme is developed utilizing interband transition for laser modulation. Using laser rate equations, more accurate predictions for the response function can be derived. Optical modulation is shown to be superior to direct modulation. In addition to this theoretical framework, first experiments are presented on the effects of illuminating a QCL with additional lasers at or above the interband gap. The first demonstration of All-Optical Modulation was achieved using time varying near infrared illumination and the complimentary signature in the MIR QCL emission was observed. In addition to extending the knowledge base of QCL research by a first calculation of its valence band structure, this work opens new possibilities in modulation and control of the QCL's MIR emission by interband transition. Application of this technique range from fundamental physics research (e.g. electron coherence) to ultrafast communication (e.g. free-space links) and high-resolution spectroscopy.

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.

Optical nonlinearities in plasmonic metamaterials (Conference Presentation)

NASA Astrophysics Data System (ADS)

Zayats, Anatoly V.

2016-04-01

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

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

PubMed

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

2015-03-17

Ultrafast intersystem crossing (ISC) processes coupled to nuclear relaxation and solvation dynamics play a central role in the photophysics and photochemistry of a wide range of transition metal complexes. These phenomena occurring within a few hundred femtoseconds are investigated experimentally by ultrafast picosecond and femtosecond transient absorption or luminescence spectroscopies, and optical laser pump-X-ray probe techniques using picosecond and femtosecond X-ray pulses. The interpretation of ultrafast structural changes, time-resolved spectra, quantum yields, and time scales of elementary processes or transient lifetimes needs robust theoretical tools combining state-of-the-art quantum chemistry and developments in quantum dynamics for solving the electronic and nuclear problems. Multimode molecular dynamics beyond the Born-Oppenheimer approximation has been successfully applied to many small polyatomic systems. Its application to large molecules containing a transition metal atom is still a challenge because of the nuclear dimensionality of the problem, the high density of electronic excited states, and the spin-orbit coupling effects. Rhenium(I) α-diimine carbonyl complexes, [Re(L)(CO)3(N,N)](n+) are thermally and photochemically robust and highly flexible synthetically. Structural variations of the N,N and L ligands affect the spectroscopy, the photophysics, and the photochemistry of these chromophores easily incorporated into a complex environment. Visible light absorption opens the route to a wide range of applications such as sensors, probes, or emissive labels for imaging biomolecules. Halide complexes [Re(X)(CO)3(bpy)] (X = Cl, Br, or I; bpy = 2,2'-bipyridine) exhibit complex electronic structure and large spin-orbit effects that do not correlate with the heavy atom effects. Indeed, the (1)MLCT → (3)MLCT intersystem crossing (ISC) kinetics is slower than in [Ru(bpy)3](2+) or [Fe(bpy)3](2+) despite the presence of a third-row transition metal. Counterintuitively, singlet excited-state lifetime increases on going from Cl (85 fs) to Br (128 fs) and to I (152 fs). Moreover, correlation between the Re-X stretching mode and the rate of ISC is observed. In this Account, we emphasize on the role of spin-vibronic coupling on the mechanism of ultrafast ISC put in evidence in [Re(Br)(CO)3(bpy)]. For this purpose, we have developed a model Hamiltonian for solving an 11 electronic excited states multimode problem including vibronic and SO coupling within the linear vibronic coupling (LVC) approximation and the assumption of harmonic potentials. The presence of a central metal atom coupled to rigid ligands, such as α-diimine, ensures nuclear motion of small amplitudes and a priori justifies the use of the LVC model. The simulation of the ultrafast dynamics by wavepacket propagations using the multiconfiguration time-dependent Hartree (MCTDH) method is based on density functional theory (DFT), and its time-dependent extension to excited states (TD-DFT) electronic structure data. We believe that the interplay between time-resolved experiments and these pioneering simulations covering the first picoseconds and including spin-vibronic coupling will promote a number of quantum dynamical studies that will contribute to a better understanding of ultrafast processes in a wide range of organic and inorganic chromophores easily incorporated in biosystems or supramolecular devices for specific functions.

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

NASA Astrophysics Data System (ADS)

Yu, Yi-Zhong

1995-01-01

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

Ultrafast Dynamics of Energetic Materials

DTIC Science & Technology

2014-01-23

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

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

NASA Astrophysics Data System (ADS)

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

2017-06-01

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

Mitigating intrinsic defects and laser damage using pulsetrain-burst (>100 MHz) ultrafast laser processing

NASA Astrophysics Data System (ADS)

McKinney, Luke; Frank, Felix; Graper, David; Dean, Jesse; Forrester, Paul; Rioblanc, Maxence; Nantel, Marc; Marjoribanks, Robin

2005-09-01

Ultrafast-laser micromachining has promise as an approach to trimming and 'healing' small laser-produced damage sites in laser-system optics--a common experience in state-of-the-art high-power laser systems. More-conventional approaches currently include mechanical micromachining, chemical modification, and treatment using cw and long-pulse lasers. Laser-optics materials of interest include fused silica, multilayer dielectric stacks for anti-reflection coatings or high-reflectivity mirrors, and inorganic crystals such as KD*P, used for Pockels cells and frequency-doubling. We report on novel efforts using ultrafast-laser pulsetrain-burst processing (microsecond bursts at 133 MHz) to mitigate damage in fused silica, dielectric coatings, and KD*P crystals. We have established the characteristics of pulsetrain-burst micromachining in fused silica, multilayer mirrors, and KD*P, and determined the etch rates and morphology under different conditions of fluence-delivery. From all of these, we have begun to identify new means to optimize the laser-repair of optics defects and damage.

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

PubMed

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

2016-11-01

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

Modern applications of terahertz emission spectroscopy

NASA Astrophysics Data System (ADS)

Harrel, Shayne Matthew

Terahertz (THz) emission spectroscopy (TES) is newly developed experimental technique capable of measuring ultrafast dynamics in a variety of systems. Unlike pump-probe spectroscopies where the signals are obtained indirectly, the THz waveform emitted by the dynamical process serves as the signal field. Information about processes involving a time-dependent magnetization, polarization or current is obtained using TES. The detection scheme is polarization sensitive and allows the direction of the dynamical event to be recovered. The role of solvation on intramolecular charge transfer in DMANS (4-(dimethylamino)-4'-nitrostilbene) is studied using TES in three solvents: benzene, toluene, and 1,3-dichlorobenzene. These solvents have similar molecular structures but different polarities and dielectric constants. The charge transfer dynamics are found to depend on the solvent. A secondary feature in the THz emission appearing 4-6 Ps after the main pulse provides evidence that DMANS may undergo a twisted intramolecular charge transfer state (TICT) upon photoexcitation. The ultrafast magnetization dynamics of polycrystalline Ni and single Fe films ranging in thickness from 5 nm to 60 nm are reported using TES. For samples thicker than the visible optical skin depth, (˜10 nm for Ni and ˜27 nm for Fe), the emission is easily interpreted using Lenz's law. For films thinner than visible optical skin depth, the emission patterns are qualitatively different. These results suggest that there are two generation mechanisms at work: one that arises purely from bulk demagnetization in the thick sample limit and another that is the result of difference frequency generation enhanced by the magnetized surface. A comparative study of the magnetization dynamics of a 40 nm Ni and 40 Fe film shows that the magnetization recovers faster in Fe than in Ni. The dependence of optical rectification and shift currents in unbiased GaAs (111) is reported using TES. It is found that the dependence of the emission with respect to linear excitation polarization is well described by theory. The emission with respect to elliptical polarization also agrees well with theory when exciting below and far above the bandgap. However, the THz emission when exciting slightly above the bandgap is strongly influenced by spin-polarized electrons. The magnetic field generated by these spin-polarized electrons is responsible for altering their own trajectories via the self-induced Hall effect. The dependence of THz generation mechanisms in ZnTe (110) on excitation intensity is investigated using TES. Optical rectification is found to be the dominant generation mechanism only at the lowest excitation powers (<5 mW). A model of second harmonic induced shift currents generating THz radiation is unable to explain the emissions at higher excitation powers.

Tuning optical absorption and photoexcited recombination dynamics in La1-xSrxFeO3-δ through A-site substitution and oxygen vacancies

NASA Astrophysics Data System (ADS)

Smolin, Sergey; Scafetta, Mark; Choquette, Amber; Sfeir, Matthew; Baxter, Jason; May, Steven

We study optical absorption and recombination dynamics in La1-xSrxFeO3-δ thin films, uncovering the effects of tuning nominal Fe valence via A-site substitution and oxygen stoichiometry. Variable angle spectroscopic ellipsometry was used to measure static optical properties, revealing a linear increase in absorption coefficient at 1.25 eV and a red-shifting of the optical absorption edge with increasing Sr fraction. The absorption spectra can be similarly tuned through the introduction of oxygen vacancies, indicating the critical role that nominal Fe valence plays in optical absorption. Dynamic optoelectronic properties were studied with ultrafast transient reflectance spectroscopy, revealing similar nanosecond photoexcited carrier lifetimes for oxygen deficient and stoichiometric films with the same nominal Fe valence. These results demonstrate that while the static optical absorption is strongly dependent on Fe valence tuned through cation or anion stoichiometry, oxygen vacancies do not appear to play a significantly detrimental role in the recombination kinetics. Nsf: ECCS-1201957, MRI DMR-0922929, MRI DMR-1040166. This research used resources of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science Facility, at Brookhaven National Laboratory under Contract No. DE-SC0012704.

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

DOE PAGES

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

2018-04-27

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

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

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

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

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

H.sub.2O doped WO.sub.3, ultra-fast, high-sensitivity hydrogen sensors

DOEpatents

Liu, Ping [Denver, CO; Tracy, C Edwin [Golden, CO; Pitts, J Roland [Lakewood, CO; Lee, Se-Hee [Lakewood, CO

2011-03-22

An ultra-fast response, high sensitivity structure for optical detection of low concentrations of hydrogen gas, comprising: a substrate; a water-doped WO.sub.3 layer coated on the substrate; and a palladium layer coated on the water-doped WO.sub.3 layer.

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

PubMed

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

2018-06-13

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

Photoisomerization and photoionization of the photoactive yellow protein chromophore in solution.

PubMed

Larsen, Delmar S; Vengris, Mikas; van Stokkum, Ivo H M; van der Horst, Michael A; de Weerd, Frank L; Hellingwerf, Klaas J; van Grondelle, Rienk

2004-04-01

Dispersed pump-dump-probe spectroscopy has the ability to characterize and identify the underlying ultrafast dynamical processes in complicated chemical and biological systems. This technique builds on traditional pump-probe techniques by exploring both ground- and excited-state dynamics and characterizing the connectivity between constituent transient states. We have used the dispersed pump-dump-probe technique to investigate the ground-state dynamics and competing excited-state processes in the excitation-induced ultrafast dynamics of thiomethyl p-coumaric acid, a model chromophore for the photoreceptor photoactive yellow protein. Our results demonstrate the parallel formation of two relaxation pathways (with multiple transient states) that jointly lead to two different types of photochemistry: cis-trans isomerization and detachment of a hydrated electron. The relative transition rates and quantum yields of both pathways have been determined. We find that the relaxation of the photoexcited chromophores involves multiple, transient ground-state intermediates and the chromophore in solution does not generate persistent photoisomerized products, but instead undergoes photoionization resulting in the generation of detached electrons and radicals. These results are of great value in interpreting the more complex dynamical changes in the optical properties of the photoactive yellow protein.

Photoisomerization and Photoionization of the Photoactive Yellow Protein Chromophore in Solution

PubMed Central

Larsen, Delmar S.; Vengris, Mikas; van Stokkum, Ivo H. M.; van der Horst, Michael A.; de Weerd, Frank L.; Hellingwerf, Klaas J.; van Grondelle, Rienk

2004-01-01

Dispersed pump-dump-probe spectroscopy has the ability to characterize and identify the underlying ultrafast dynamical processes in complicated chemical and biological systems. This technique builds on traditional pump-probe techniques by exploring both ground- and excited-state dynamics and characterizing the connectivity between constituent transient states. We have used the dispersed pump-dump-probe technique to investigate the ground-state dynamics and competing excited-state processes in the excitation-induced ultrafast dynamics of thiomethyl p-coumaric acid, a model chromophore for the photoreceptor photoactive yellow protein. Our results demonstrate the parallel formation of two relaxation pathways (with multiple transient states) that jointly lead to two different types of photochemistry: cis-trans isomerization and detachment of a hydrated electron. The relative transition rates and quantum yields of both pathways have been determined. We find that the relaxation of the photoexcited chromophores involves multiple, transient ground-state intermediates and the chromophore in solution does not generate persistent photoisomerized products, but instead undergoes photoionization resulting in the generation of detached electrons and radicals. These results are of great value in interpreting the more complex dynamical changes in the optical properties of the photoactive yellow protein. PMID:15041690

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.

Dynamical anisotropic response of black phosphorus under magnetic field

NASA Astrophysics Data System (ADS)

Liu, Xuefeng; Lu, Wei; Zhou, Xiaoying; Zhou, Yang; Zhang, Chenglong; Lai, Jiawei; Ge, Shaofeng; Sekhar, M. Chandra; Jia, Shuang; Chang, Kai; Sun, Dong

2018-04-01

Black phosphorus (BP) has emerged as a promising material candidate for next generation electronic and optoelectronic devices due to its high mobility, tunable band gap and highly anisotropic properties. In this work, polarization resolved ultrafast mid-infrared transient reflection spectroscopy measurements are performed to study the dynamical anisotropic optical properties of BP under magnetic fields up to 9 T. The relaxation dynamics of photoexcited carrier is found to be insensitive to the applied magnetic field due to the broadening of the Landau levels and large effective mass of carriers. While the anisotropic optical response of BP decreases with increasing magnetic field, its enhancement due to the excitation of hot carriers is similar to that without magnetic field. These experimental results can be well interpreted by the magneto-optical conductivity of the Landau levels of BP thin film, based on an effective k · p Hamiltonian and linear response theory. These findings suggest attractive possibilities of multi-dimensional control of anisotropic response (AR) of BP with light, electric and magnetic field, which further introduces BP to the fantastic magnetic field sensitive applications.

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.

Synthesis of Dibenzo[hi,st]ovalene and Its Amplified Spontaneous Emission in a Polystyrene Matrix.

PubMed

Paternò, Giuseppe M; Chen, Qiang; Wang, Xiao-Ye; Liu, Junzhi; Motti, Silvia G; Petrozza, Annamaria; Feng, Xinliang; Lanzani, Guglielmo; Müllen, Klaus; Narita, Akimitsu; Scotognella, Francesco

2017-06-06

A large number of graphene molecules, or large polycyclic aromatic hydrocarbons (PAHs), have been synthesized and display various optoelectronic properties. Nevertheless, their potential for application in photonics has remained largely unexplored. Herein, we describe the synthesis of a highly luminescent and stable graphene molecule, namely a substituted dibenzo[hi,st]ovalene (DBO 1), with zigzag edges and elucidate its promising optical-gain properties by means of ultrafast transient absorption spectroscopy. Upon incorporation of DBO into an inert polystyrene matrix, amplified stimulated emission can be observed with a relatively low power threshold (ca. 60 μJ cm -2 ), thus highlighting its high potential for lasing applications. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Single Broadband Phase-Shaped Pulse Stimulated Raman Spectroscopy for Standoff Trace Explosive Detection.

PubMed

Glenn, Rachel; Dantus, Marcos

2016-01-07

Recent success with trace explosives detection based on the single ultrafast pulse excitation for remote stimulated Raman scattering (SUPER-SRS) prompts us to provide new results and a Perspective that describes the theoretical foundation of the strategy used for achieving the desired sensitivity and selectivity. SUPER-SRS provides fast and selective imaging while being blind to optical properties of the substrate such as color, texture, or laser speckle. We describe the strategy of combining coherent vibrational excitation with a reference pulse in order to detect stimulated Raman gain or loss. A theoretical model is used to reproduce experimental spectra and to determine the ideal pulse parameters for best sensitivity, selectivity, and resolution when detecting one or more compounds simultaneously.

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

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

Ultrafast spectroscopy reveals subnanosecond peptide conformational dynamics and validates molecular dynamics simulation

NASA Astrophysics Data System (ADS)

Spörlein, Sebastian; Carstens, Heiko; Satzger, Helmut; Renner, Christian; Behrendt, Raymond; Moroder, Luis; Tavan, Paul; Zinth, Wolfgang; Wachtveitl, Josef

2002-06-01

Femtosecond time-resolved spectroscopy on model peptides with built-in light switches combined with computer simulation of light-triggered motions offers an attractive integrated approach toward the understanding of peptide conformational dynamics. It was applied to monitor the light-induced relaxation dynamics occurring on subnanosecond time scales in a peptide that was backbone-cyclized with an azobenzene derivative as optical switch and spectroscopic probe. The femtosecond spectra permit the clear distinguishing and characterization of the subpicosecond photoisomerization of the chromophore, the subsequent dissipation of vibrational energy, and the subnanosecond conformational relaxation of the peptide. The photochemical cis/trans-isomerization of the chromophore and the resulting peptide relaxations have been simulated with molecular dynamics calculations. The calculated reaction kinetics, as monitored by the energy content of the peptide, were found to match the spectroscopic data. Thus we verify that all-atom molecular dynamics simulations can quantitatively describe the subnanosecond conformational dynamics of peptides, strengthening confidence in corresponding predictions for longer time scales.

Clocking Femtosecond Collisional Dynamics via Resonant X-Ray Spectroscopy

NASA Astrophysics Data System (ADS)

van den Berg, Q. Y.; Fernandez-Tello, E. V.; Burian, T.; Chalupský, J.; Chung, H.-K.; Ciricosta, O.; Dakovski, G. L.; Hájková, V.; Hollebon, P.; Juha, L.; Krzywinski, J.; Lee, R. W.; Minitti, M. P.; Preston, T. R.; de la Varga, A. G.; Vozda, V.; Zastrau, U.; Wark, J. S.; Velarde, P.; Vinko, S. M.

2018-02-01

Electron-ion collisional dynamics is of fundamental importance in determining plasma transport properties, nonequilibrium plasma evolution, and electron damage in diffraction imaging applications using bright x-ray free-electron lasers (FELs). Here we describe the first experimental measurements of ultrafast electron impact collisional ionization dynamics using resonant core-hole spectroscopy in a solid-density magnesium plasma, created and diagnosed with the Linac Coherent Light Source x-ray FEL. By resonantly pumping the 1 s →2 p transition in highly charged ions within an optically thin plasma, we have measured how off-resonance charge states are populated via collisional processes on femtosecond time scales. We present a collisional cross section model that matches our results and demonstrates how the cross sections are enhanced by dense-plasma effects including continuum lowering. Nonlocal thermodynamic equilibrium collisional radiative simulations show excellent agreement with the experimental results and provide new insight on collisional ionization and three-body-recombination processes in the dense-plasma regime.

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

Clocking Femtosecond Collisional Dynamics via Resonant X-Ray Spectroscopy

DOE PAGES

van den Berg, Q. Y.; Fernandez-Tello, E. V.; Burian, T.; ...

2018-02-01

Electron-ion collisional dynamics is of fundamental importance in determining plasma transport properties, nonequilibrium plasma evolution, and electron damage in diffraction imaging applications using bright x-ray free-electron lasers (FELs). Here in this paper, we describe the first experimental measurements of ultrafast electron impact collisional ionization dynamics using resonant core-hole spectroscopy in a solid-density magnesium plasma, created and diagnosed with the Linac Coherent Light Source x-ray FEL. By resonantly pumping the 1s → 2p transition in highly charged ions within an optically thin plasma, we have measured how off-resonance charge states are populated via collisional processes on femtosecond time scales. We presentmore » a collisional cross section model that matches our results and demonstrates how the cross sections are enhanced by dense-plasma effects including continuum lowering. Nonlocal thermodynamic equilibrium collisional radiative simulations show excellent agreement with the experimental results and provide new insight on collisional ionization and three-body-recombination processes in the dense-plasma regime.« less

Electron phonon couplings in 2D perovskite probed by ultrafast photoinduced absorption spectroscopy

NASA Astrophysics Data System (ADS)

Huynh, Uyen; Ni, Limeng; Rao, Akshay

We use the time-resolved photoinduced absorption (PIA) spectroscopy with 20fs time resolution to investigate the electron phonon coupling in the self-assembled hybrid organic layered perovskite, the hexyl ammonium lead iodide compound (C6H13NH3)2 (PbI4) . The coupling results in the broadening and asymmetry of its temperature-dependence photoluminescence spectra. The exact time scale of this coupling, however, wasn't reported experimentally. Here we show that using an ultrashort excitation pulse allows us to resolve from PIA kinetics the oscillation of coherent longitudinal optical phonons that relaxes and self-traps electrons to lower energy states within 200 fs. The 200fs relaxation time is equivalent to a coupling strength of 40meV. Two coupled phonon modes are also identified as about 100 cm-1 and 300 cm-1 from the FFT spectrum of the PIA kinetics. The lower energy mode is consistent with previous reports and Raman spectrum but the higher energy one hasn't been observed before.

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

NASA Astrophysics Data System (ADS)

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

2009-11-01

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

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

Tunable near- to mid-infrared pump terahertz probe spectroscopy in reflection geometry

NASA Astrophysics Data System (ADS)

Zhang, S. J.; Wang, Z. X.; Dong, T.; Wang, N. L.

2017-10-01

Strong-field mid-infrared pump-terahertz (THz) probe spectroscopy has been proven as a powerful tool for light control of different orders in strongly correlated materials. We report the construction of an ultrafast broadband infrared pump-THz probe system in reflection geometry. A two-output optical parametric amplifier is used for generating mid-infrared pulses with GaSe as the nonlinear crystal. The setup is capable of pumping bulk materials at wavelengths ranging from 1.2 μm to 15 μm and beyond, and detecting the subtle, transient photoinduced changes in the reflected electric field of the THz probe at different temperatures. As a demonstration, we present 15 μm pump-THz probe measurements of a bulk EuSbTe3 single crystal. A 0:5% transient change in the reflected THz electric field can be clearly resolved. The widely tuned pumping energy could be used in mode-selective excitation experiments and applied to many strongly correlated electron systems.

Broadband two-dimensional electronic spectroscopy in an actively phase stabilized pump-probe configuration.

PubMed

Zhu, Weida; Wang, Rui; Zhang, Chunfeng; Wang, Guodong; Liu, Yunlong; Zhao, Wei; Dai, Xingcan; Wang, Xiaoyong; Cerullo, Giulio; Cundiff, Steven; Xiao, Min

2017-09-04

We introduce a novel configuration for two-dimensional electronic spectroscopy (2DES) that combines the partially collinear pump-probe geometry with active phase locking. We demonstrate the method on a solution sample of CdSe/ZnS nanocrystals by employing two non-collinear optical parametric amplifiers as the pump and probe sources. The two collinear pump pulse replicas are created using a Mach-Zehnder interferometer phase stabilized by active feedback electronics. Taking the advantage of separated paths of the two pump pulses in the interferometer, we improve the signal-to-noise ratio with double modulation of the individual pump beams. In addition, a quartz wedge pair manipulates the phase difference between the two pump pulses, enabling the recovery of the rephasing and non-rephasing signals. Our setup integrates many advantages of available 2DES techniques with robust phase stabilization, ultrafast time resolution, two-color operation, long delay scan, individual polarization manipulation and the ease of implementation.

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.

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

NASA Astrophysics Data System (ADS)

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

2018-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-06-01

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

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

PubMed Central

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

2017-01-01

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

Visualization of carrier dynamics in p(n)-type GaAs by scanning ultrafast electron microscopy

PubMed Central

Cho, Jongweon; Hwang, Taek Yong; Zewail, Ahmed H.

2014-01-01

Four-dimensional scanning ultrafast electron microscopy is used to investigate doping- and carrier-concentration-dependent ultrafast carrier dynamics of the in situ cleaved single-crystalline GaAs(110) substrates. We observed marked changes in the measured time-resolved secondary electrons depending on the induced alterations in the electronic structure. The enhancement of secondary electrons at positive times, when the electron pulse follows the optical pulse, is primarily due to an energy gain involving the photoexcited charge carriers that are transiently populated in the conduction band and further promoted by the electron pulse, consistent with a band structure that is dependent on chemical doping and carrier concentration. When electrons undergo sufficient energy loss on their journey to the surface, dark contrast becomes dominant in the image. At negative times, however, when the electron pulse precedes the optical pulse (electron impact), the dynamical behavior of carriers manifests itself in a dark contrast which indicates the suppression of secondary electrons upon the arrival of the optical pulse. In this case, the loss of energy of material’s electrons is by collisions with the excited carriers. These results for carrier dynamics in GaAs(110) suggest strong carrier–carrier scatterings which are mirrored in the energy of material’s secondary electrons during their migration to the surface. The approach presented here provides a fundamental understanding of materials probed by four-dimensional scanning ultrafast electron microscopy, and offers possibilities for use of this imaging technique in the study of ultrafast charge carrier dynamics in heterogeneously patterned micro- and nanostructured material surfaces and interfaces. PMID:24469803

Visualization of carrier dynamics in p(n)-type GaAs by scanning ultrafast electron microscopy.

PubMed

Cho, Jongweon; Hwang, Taek Yong; Zewail, Ahmed H

2014-02-11

Four-dimensional scanning ultrafast electron microscopy is used to investigate doping- and carrier-concentration-dependent ultrafast carrier dynamics of the in situ cleaved single-crystalline GaAs(110) substrates. We observed marked changes in the measured time-resolved secondary electrons depending on the induced alterations in the electronic structure. The enhancement of secondary electrons at positive times, when the electron pulse follows the optical pulse, is primarily due to an energy gain involving the photoexcited charge carriers that are transiently populated in the conduction band and further promoted by the electron pulse, consistent with a band structure that is dependent on chemical doping and carrier concentration. When electrons undergo sufficient energy loss on their journey to the surface, dark contrast becomes dominant in the image. At negative times, however, when the electron pulse precedes the optical pulse (electron impact), the dynamical behavior of carriers manifests itself in a dark contrast which indicates the suppression of secondary electrons upon the arrival of the optical pulse. In this case, the loss of energy of material's electrons is by collisions with the excited carriers. These results for carrier dynamics in GaAs(110) suggest strong carrier-carrier scatterings which are mirrored in the energy of material's secondary electrons during their migration to the surface. The approach presented here provides a fundamental understanding of materials probed by four-dimensional scanning ultrafast electron microscopy, and offers possibilities for use of this imaging technique in the study of ultrafast charge carrier dynamics in heterogeneously patterned micro- and nanostructured material surfaces and interfaces.

Femtosecond optical characterization and applications in cadmium(manganese) telluride diluted magnetic semiconductors

NASA Astrophysics Data System (ADS)

Wang, Daozhi

This thesis is devoted to the optical characterization of Cd(Mn)Te single crystals. I present the studies of free-carrier dynamics and generation and detection of coherent acoustic phonons (CAPS) using time-resolved femtosecond pump-probe spectroscopy. The giant Faraday effect and ultrafast responsivity of Cd(Mn)Te to sub-picosecond electromagnetic transients are also demonstrated and discussed in detail. The first, few-picosecond-long electronic process after the initial optical excitation exhibits very distinct characteristic dependence on the excitation condition, and in case of Cd(Mn)Te, it has been attributed to the collective effects of band filling, band renormalization, and two-photon absorption. A closed-form, analytic expression for the differential reflectivity induced by the CAPs is derived based on the propagating-strain-pulse model and it accounts very well for our experimental observations. The accurate values of the Mn concentration and longitudinal sound velocity nu s in Cd(Mn)Te were obtained by fitting the data of the refractive index dependence on the probe wavelength to the Schubert model. In Cd 0.91Mn0.09Te, nus was found to be 3.6x103 m/s. Our comparison studies from the one-color and two-color experiments reveal that the intrinsic phonon lifetime in Cd(Mn)Te was at least on the order of nanoseconds, and the observed exponential damping of the CAP oscillations was due to the finite absorption depth of the probe light. Optically-induced electronic stress has been demonstrated to be the main generation mechanism of CAPs. We also present the giant Faraday effect in the Cd(Mn)Te and the spectra of the Verdet constant, which is mainly due to the exchange interaction between the Mn ions and band electrons. The spectral characteristics of the Verdet constant in Cd(Mn)Te exhibit very unique features compared to that in pure semiconductors. In our time-resolved sampling experiments at the room temperature, the response of the Cd(Mn)Te, particularly with low Mn concentrations, to the sub-picosecond electromagnetic pulses has been demonstrated for the first time and studied in detail. The physical origin of the ultrafast responsivity is shown to be the electro-optic (Pockels) effect, simultaneously excluding the magneto-optical (Faraday) effect due to the Mn-ion spin dynamics. The discrepancy between the absence of the low-frequency Pockels effect and the ultrafast sampling results, suggests that in Cd(Mn)Te crystals at low frequencies, the electric field component of the external electromagnetic transients is screened by the free carriers (holes). At very high (THz) frequencies, tested by our sampling experiment, Mn spins are too slow to respond and we observe the very large Pockels effect in Cd(Mn)Te crystals.

Photoconductive terahertz near-field detector with a hybrid nanoantenna array cavity

DOE PAGES

Mitrofanov, Oleg; Brener, Igal; Luk, Ting S.; ...

2015-11-19

Nanoscale structuring of optical materials leads to modification of their properties and can be used for improving efficiencies of photonic devices and for enabling new functionalities. In ultrafast optoelectronic switches for generation and detection of terahertz (THz) radiation, incorporation of nanostructures allows us to overcome inherent limitations of photoconductive materials. We propose and demonstrate a nanostructured photoconductive THz detector for sampling highly localized THz fields, down to the level of λ/150. The nanostructure that consists of an array of optical nanoantennas and a distributed Bragg reflector forms a hybrid cavity, which traps optical gate pulses within the photoconductive layer. Themore » effect of photon trapping is observed as enhanced absorption at a designed wavelength. This optically thin photoconductive THz detector allows us to detect highly confined evanescent THz fields coupled through a deeply subwavelength aperture as small as 2 μm (λ/150 at 1 THz). As a result, by monolithically integrating the THz detector with apertures ranging from 2 to 5 μm we realize higher spatial resolution and higher sensitivity in aperture-type THz near-field microscopy and THz time-domain spectroscopy.« less

Capturing local structure modulations of photoexcited BiVO4 by ultrafast transient XAFS.

PubMed

Uemura, Yohei; Kido, Daiki; Koide, Akihiro; Wakisaka, Yuki; Niwa, Yasuhiro; Nozawa, Shunsuke; Ichiyanagi, Kohei; Fukaya, Ryo; Adachi, Shin-Ichi; Katayama, Tetsuo; Togashi, Tadashi; Owada, Shigeki; Yabashi, Makina; Hatada, Keisuke; Iwase, Akihide; Kudo, Akihiko; Takakusagi, Satoru; Yokoyama, Toshihiko; Asakura, Kiyotaka

2017-06-29

Ultrafast excitation of photocatalytically active BiVO 4 was characterized by femto- and picosecond transient X-ray absorption fine structure spectroscopy. An initial photoexcited state (≪500 fs) changed to a metastable state accompanied by a structural change with a time constant of ∼14 ps. The structural change might stabilize holes on oxygen atoms since the interaction between Bi and O increases.

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

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

Park, Joonkyu; Zhang, Qingteng; Chen, Pice

2015-08-27

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

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

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

NASA Astrophysics Data System (ADS)

Lamour, Tobias P.; Reid, Derryck T.

2011-08-01

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

Ultrafast 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.

OSA Proceedings on Ultrafast Electronics and Optoelectronics Held in San Francisco, California on January 25 -27, 1993. Volume 14,

DTIC Science & Technology

1993-01-27

Venkatesan, Zhi- Yuan Shen, Philip Pang, Dennis J. Kountz, and William L Holstein Response of a Nb/A1203/Nb Tunnel Junction to Picosecond Electrical Pulses...Mwhra (edo) 0 1993 Optical Sockty ofAnierica 152 Ultrafast Electronics and Optoelectronics core cladding COW MAD 75. 4UHN 1058nm 50Ps A A optical...Maryland. College Park; Maryland 20742 7hi-Yuan Shen, Philip Pang, Dennis J. Kountz, and William L. Holstein Central Research and Development, Du Pont, PO

Multidimensional infrared spectroscopy reveals the vibrational and solvation dynamics of isoniazid

NASA Astrophysics Data System (ADS)

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

2015-06-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-06-01

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

Nanoscale diffractive probing of strain dynamics in ultrafast transmission electron microscopy

PubMed Central

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

2018-01-01

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

Filter-Based Dispersion-Managed Versatile Ultrafast Fibre Laser

PubMed Central

Peng, Junsong; Boscolo, Sonia

2016-01-01

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

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

PubMed

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

2018-01-01

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

Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase.

PubMed

Lu, Jian; Zhang, Yaqing; Hwang, Harold Y; Ofori-Okai, Benjamin K; Fleischer, Sharly; Nelson, Keith A

2016-10-18

Ultrafast 2D spectroscopy uses correlated multiple light-matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum; its extension to the terahertz regime of the electromagnetic spectrum, where a rich variety of material degrees of freedom reside, remains an experimental challenge. We report a demonstration of ultrafast 2D terahertz spectroscopy of gas-phase molecular rotors at room temperature. Using time-delayed terahertz pulse pairs, we observe photon echoes and other nonlinear signals resulting from molecular dipole orientation induced by multiple terahertz field-dipole interactions. The nonlinear time domain orientation signals are mapped into the frequency domain in 2D rotational spectra that reveal J-state-resolved nonlinear rotational dynamics. The approach enables direct observation of correlated rotational transitions and may reveal rotational coupling and relaxation pathways in the ground electronic and vibrational state.

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

NASA Astrophysics Data System (ADS)

Ghadrdan, Majid; Mansouri-Birjandi, Mohammad Ali

2017-11-01

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

Nonlinear ultrafast optical response in organic molecular crystals

NASA Astrophysics Data System (ADS)

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

2012-02-01

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

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

PubMed Central

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

2017-01-01

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

Femtosecond transient absorption spectroscopy of silanized silicon quantum dots

NASA Astrophysics Data System (ADS)

Kuntermann, Volker; Cimpean, Carla; Brehm, Georg; Sauer, Guido; Kryschi, Carola; Wiggers, Hartmut

2008-03-01

Excitonic properties of colloidal silicon quantum dots (Si qdots) with mean sizes of 4nm were examined using stationary and time-resolved optical spectroscopy. Chemically stable silicon oxide shells were prepared by controlled surface oxidation and silanization of HF-etched Si qdots. The ultrafast relaxation dynamics of photogenerated excitons in Si qdot colloids were studied on the picosecond time scale from 0.3psto2.3ns using femtosecond-resolved transient absorption spectroscopy. The time evolution of the transient absorption spectra of the Si qdots excited with a 150fs pump pulse at 390nm was observed to consist of decays of various absorption transitions of photoexcited electrons in the conduction band which overlap with both the photoluminescence and the photobleaching of the valence band population density. Gaussian deconvolution of the spectroscopic data allowed for disentangling various carrier relaxation processes involving electron-phonon and phonon-phonon scatterings or arising from surface-state trapping. The initial energy and momentum relaxation of hot carriers was observed to take place via scattering by optical phonons within 0.6ps . Exciton capturing by surface states forming shallow traps in the amorphous SiOx shell was found to occur with a time constant of 4ps , whereas deeper traps presumably localized in the Si-SiOx interface gave rise to exciton trapping processes with time constants of 110 and 180ps . Electron transfer from initially populated, higher-lying surface states to the conduction band of Si qdots (>2nm) was observed to take place within 400 or 700fs .

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

PubMed

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

2018-01-04

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

Real-time visualization of soliton molecules with evolving behavior in an ultrafast fiber laser

NASA Astrophysics Data System (ADS)

Liu, Meng; Li, Heng; Luo, Ai-Ping; Cui, Hu; Xu, Wen-Cheng; Luo, Zhi-Chao

2018-03-01

Ultrafast fiber lasers have been demonstrated to be great platforms for the investigation of soliton dynamics. The soliton molecules, as one of the most fascinating nonlinear phenomena, have been a hot topic in the field of nonlinear optics in recent years. Herein, we experimentally observed the real-time evolving behavior of soliton molecule in an ultrafast fiber laser by using the dispersive Fourier transformation technology. Several types of evolving soliton molecules were obtained in our experiments, such as soliton molecules with monotonically or chaotically evolving phase, flipping and hopping phase. These results would be helpful to the communities interested in soliton nonlinear dynamics as well as ultrafast laser technologies.

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

PubMed

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

2018-05-03

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

Ultrafast Microfluidic Cellular Imaging by Optical Time-Stretch.

PubMed

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

2016-01-01

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

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.

Optical characterization of shock-induced chemistry in the explosive nitromethane using DFT and time-dependent DFT

NASA Astrophysics Data System (ADS)

Pellouchoud, Lenson; Reed, Evan

2014-03-01

With continual improvements in ultrafast optical spectroscopy and new multi-scale methods for simulating chemistry for hundreds of picoseconds, the opportunity is beginning to exist to connect experiments with simulations on the same timescale. We compute the optical properties of the liquid phase energetic material nitromethane (CH3NO2) for the first 100 picoseconds behind the front of a simulated shock at 6.5km/s, close to the experimentally observed detonation shock speed. We utilize molecular dynamics trajectories computed using the multi-scale shock technique (MSST) for time-resolved optical spectrum calculations based on both linear response time-dependent DFT (TDDFT) and the Kubo-Greenwood (KG) formula within Kohn-Sham DFT. We find that TDDFT predicts optical conductivities 25-35% lower than KG-based values and provides better agreement with the experimentally measured index of refraction of unreacted nitromethane. We investigate the influence of electronic temperature on the KG spectra and find no significant effect at optical wavelengths. With all methods, the spectra evolve non-monotonically in time as shock-induced chemistry takes place. We attribute the time-resolved absorption at optical wavelengths to time-dependent populations of molecular decomposition products, including NO, CNO, CNOH, H2O, and larger molecules. Supported by NASA Space Technology Research Fellowship (NSTRF) #NNX12AM48H.

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

PubMed

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

2013-10-07

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

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

NASA Astrophysics Data System (ADS)

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

2017-11-01

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

Ultrafast dynamics of an unoccupied surface resonance state in B i2T e2Se

NASA Astrophysics Data System (ADS)

Munisa, Nurmamat; Krasovskii, E. E.; Ishida, Y.; Sumida, K.; Chen, Jiahua; Yoshikawa, T.; Chulkov, E. V.; Kokh, K. A.; Tereshchenko, O. E.; Shin, S.; Kimura, Akio

2018-03-01

Electronic structure and electron dynamics in the ternary topological insulator B i2T e2Se are studied with time- and angle-resolved photoemission spectroscopy using optical pumping. An unoccupied surface resonance split off from the bulk conduction band previously indirectly observed in scanning tunneling measurements is spectroscopically identified. Furthermore, an unoccupied topological surface state (TSS) is found, which is serendipitously located at about 1.5 eV above the occupied TSS, thereby facilitating direct optical transitions between the two surface states at ℏ ω =1.5 eV in an n -type topological insulator. An appreciable nonequilibrium population of the bottom of the bulk conduction band is observed for longer than 15 ps after the pump pulse. This leads to a long recovery time of the lower TSS, which is constantly populated by the electrons coming from the bulk conduction band. Our results demonstrate B i2T e2Se to be an ideal platform for designing future optoelectronic devices based on 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

Exploring Ultrafast Structural Dynamics for Energetic Enhancement or Disruption

DTIC Science & Technology

2016-03-01

it. In a pump -push/ dump probe experiment, a secondary laser pulse (push/ dump ) is used after the initial perturbation due to the pump pulse. The...increased. The pump -push/ dump probe technique is a difficult experiment that requires a highly stable laser source. Ultrafast pump -probe experiments...decomposition of solids. Journal of Applied Physics. 2001;89:4156–4166. 17. Kee TW. Femtosecond pump -push-probe and pump - dump -probe spectroscopy of

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

PubMed

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

2018-04-30

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

An ultrafast electron microscope gun driven by two-photon photoemission from a nanotip cathode

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

Bormann, Reiner; Strauch, Stefanie; Schäfer, Sascha, E-mail: schaefer@ph4.physik.uni-goettingen.de

We experimentally and numerically investigate the performance of an advanced ultrafast electron source, based on two-photon photoemission from a tungsten needle cathode incorporated in an electron microscope gun geometry. Emission properties are characterized as a function of the electrostatic gun settings, and operating conditions leading to laser-triggered electron beams of very low emittance (below 20 nm mrad) are identified. The results highlight the excellent suitability of optically driven nano-cathodes for the further development of ultrafast transmission electron microscopy.

Cross-phase modulation bandwidth in ultrafast fiber wavelength converters

NASA Astrophysics Data System (ADS)

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

2006-12-01

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

Acousto-Optic Tunable Filter for Time-Domain Processing of Ultra-Short Optical Pulses,

DTIC Science & Technology

The application of acousto - optic tunable filters for shaping of ultra-fast pulses in the time domain is analyzed and demonstrated. With the rapid...advance of acousto - optic tunable filter (AOTF) technology, the opportunity for sophisticated signal processing capabilities arises. AOTFs offer unique

Ultrafast Plasmonic Control of Second Harmonic Generation

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

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

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

Ultrafast Plasmonic Control of Second Harmonic Generation

DOE PAGES

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

2016-06-01

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

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

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

NASA Astrophysics Data System (ADS)

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

2017-04-01

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

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

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

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

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

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

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

DOE PAGES

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

2017-12-24

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

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

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

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

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

Phosphorene quantum dot saturable absorbers for ultrafast fiber lasers

PubMed Central

Du, J.; Zhang, M.; Guo, Z.; Chen, J.; Zhu, X.; Hu, G.; Peng, P.; Zheng, Z.; Zhang, H.

2017-01-01

We fabricate ultrasmall phosphorene quantum dots (PQDs) with an average size of 2.6 ± 0.9 nm using a liquid exfoliation method involving ultrasound probe sonication followed by bath sonication. By coupling the as-prepared PQDs with microfiber evanescent light field, the PQD-based saturable absorber (SA) device exhibits ultrafast nonlinear saturable absorption property, with an optical modulation depth of 8.1% at the telecommunication band. With the integration of the all-fiber PQD-based SA, a continuous-wave passively mode-locked erbium-doped (Er-doped) laser cavity delivers stable, self-starting pulses with a pulse duration of 0.88 ps and at the cavity repetition rate of 5.47 MHz. Our results contribute to the growing body of work studying the nonlinear optical properties of ultrasmall PQDs that present new opportunities of this two-dimensional (2D) nanomaterial for future ultrafast photonic technologies. PMID:28211471

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

PubMed

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

2018-03-15

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

Realizing high-quality ultralarge momentum states and ultrafast topological transitions using semiconductor hyperbolic metamaterials

DOE PAGES

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

2015-08-05

We employ both the effective medium approximation (EMA) and Bloch theory to compare the dispersion properties of semiconductor hyperbolic metamaterials (SHMs) at mid-infrared frequencies and metallic hyperbolic metamaterials (MHMs) at visible frequencies. This analysis reveals the conditions under which the EMA can be safely applied for both MHMs and SHMs. We find that the combination of precise nanoscale layering and the longer infrared operating wavelengths puts the SHMs well within the effective medium limit and, in contrast to MHMs, allows for the attainment of very high photon momentum states. Additionally, SHMs allow for new phenomena such as ultrafast creation ofmore » the hyperbolic manifold through optical pumping. Furthermore, we examine the possibility of achieving ultrafast topological transitions through optical pumping which can photo-dope appropriately designed quantum wells on the femtosecond time scale.« less

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

NASA Astrophysics Data System (ADS)

Islam, Md Mahbubul; Strachan, Alejandro

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

Versatile multi-wavelength ultrafast fiber laser mode-locked by carbon nanotubes

PubMed Central

Liu, Xueming; Han, Dongdong; Sun, Zhipei; Zeng, Chao; Lu, Hua; Mao, Dong; Cui, Yudong; Wang, Fengqiu

2013-01-01

Multi-wavelength lasers have widespread applications (e.g. fiber telecommunications, pump-probe measurements, terahertz generation). Here, we report a nanotube-mode-locked all-fiber ultrafast oscillator emitting three wavelengths at the central wavelengths of about 1540, 1550, and 1560 nm, which are tunable by stretching fiber Bragg gratings. The output pulse duration is around 6 ps with a spectral width of ~0.5 nm, agreeing well with the numerical simulations. The triple-laser system is controlled precisely and insensitive to environmental perturbations with <0.04% amplitude fluctuation. Our method provides a simple, stable, low-cost, multi-wavelength ultrafast-pulsed source for spectroscopy, biomedical research and telecommunications. PMID:24056500

Femtochemistry of confined water

NASA Astrophysics Data System (ADS)

Douhal, A.; Carranza, M. A.; Sanz, M.; Organero, J. A.; Santos, L.

In this contribution, we applied ultrafast spectroscopy to study the H-bond network of water confined in nanostructures (Cyclodextrins and Micelles). We examine the effect of caging on ultrafast reaction dynamics and discuss the related processes under different experimental conditions. The results show an ultrafast dynamic giving birth to intermediates of the probe, which show femtosecond and picosecond dynamics leading to the final structure at the excited state. The results show the high sensitivity of the used technique in detecting small of water. This work was supported by the Ministry of Science and Technology (MCYT, Spain) and ``Conserjería de Ciencia y Tecnologia de la JCCM, Spain'' through projects MAT2002-01829 and PAI-02-004.

Real-Time Time-Frequency Two-Dimensional Imaging of Ultrafast Transient Signals in Solid-State Organic Materials

PubMed Central

Takeda, Jun; Ishida, Akihiro; Makishima, Yoshinori; Katayama, Ikufumi

2010-01-01

In this review, we demonstrate a real-time time-frequency two-dimensional (2D) pump-probe imaging spectroscopy implemented on a single shot basis applicable to excited-state dynamics in solid-state organic and biological materials. Using this technique, we could successfully map ultrafast time-frequency 2D transient absorption signals of β-carotene in solid films with wide temporal and spectral ranges having very short accumulation time of 20 ms per unit frame. The results obtained indicate the high potential of this technique as a powerful and unique spectroscopic tool to observe ultrafast excited-state dynamics of organic and biological materials in solid-state, which undergo rapid photodegradation. PMID:22399879

QoS support over ultrafast TDM optical networks

NASA Astrophysics Data System (ADS)

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

1999-08-01

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

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.

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.

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

NASA Astrophysics Data System (ADS)

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

2015-05-01

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

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

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

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

2014-07-01

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

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

NASA Astrophysics Data System (ADS)

Engelhorn, Kyle Craig

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

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

NASA Astrophysics Data System (ADS)

Yang, Chuan; Zhang, Haibin

2017-03-01

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

Multiple exciton dissociation in CdSe quantum dots by ultrafast electron transfer to adsorbed methylene blue.

PubMed

Huang, Jier; Huang, Zhuangqun; Yang, Ye; Zhu, Haiming; Lian, Tianquan

2010-04-07

Multiexciton generation in quantum dots (QDs) may provide a new approach for improving the solar-to-electric power conversion efficiency in QD-based solar cells. However, it remains unclear how to extract these excitons before the ultrafast exciton-exciton annihilation process. In this study we investigate multiexciton dissociation dynamics in CdSe QDs adsorbed with methylene blue (MB(+)) molecules by transient absorption spectroscopy. We show that excitons in QDs dissociate by ultrafast electron transfer to MB(+) with an average time constant of approximately 2 ps. The charge separated state is long-lived (>1 ns), and the charge recombination rate increases with the number of dissociated excitons. Up to three MB(+) molecules per QD can be reduced by exciton dissociation. Our result demonstrates that ultrafast interfacial charge separation can effectively compete with exciton-exciton annihilation, providing a viable approach for utilizing short-lived multiple excitons in QDs.

Ultrafast fluorescence spectroscopy via upconversion applications to biophysics.

PubMed

Xu, Jianhua; Knutson, Jay R

2008-01-01

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

A dynamic and ultrafast group delay tuning mechanism in two microcavities side-coupled with a waveguide system

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

Wang, Boyun; Wang, Tao, E-mail: wangtao@hust.edu.cn; Tang, Jian

2014-10-07

We theoretically propose a dynamic and ultrafast group delay tuning mechanism in two microcavities side-coupled to a waveguide system through external optical pump beams. The optical Kerr effect modulation method is applied to improve tuning rate with response time of subpicoseconds or even femtoseconds. The group delay of an all-optical analog to electromagnetically induced transparency effect can be controlled by tuning either the frequency of photonic crystal microcavities or the propagation phase of line waveguide. Group delay is controlled between 5.88 and 70.98 ps by dynamically tuning resonant frequencies of the microcavities. Alternatively, the group delay is controlled between 1.86more » and 12.08 ps by dynamically tuning the propagation phase of line waveguide. All observed schemes are analyzed rigorously through finite-difference time-domain simulations and coupled-mode formalism. Results show a new direction toward microstructure integration optical pulse trapping and all-optical dynamical storage of light devices in optical communication and quantum information processing.« less

Static and dynamic optical properties of La 1-xSr xFeO 3-δ: The effects of A-site and oxygen stoichiometry

DOE PAGES

Sergey Y. Smolin; Sfeir, Matthew Y.; Scafetta, Mark D.; ...

2015-12-09

Perovskite oxides are a promising material class for photovoltaic and photocatalytic applications due to their visible band gaps, nanosecond recombination lifetimes, and great chemical diversity. However, there is limited understanding of the link between composition and static and dynamic optical properties, despite the critical role these properties play in the design of light-harvesting devices. To clarify these relationships, we systemically studied the optoelectronic properties in La 1-xSr xFeO 3-δ epitaxial films, uncovering the effects of A-site cation substitution and oxygen stoichiometry. Variable-angle spectroscopic ellipsometry was used to measure static optical properties, revealing a linear increase in absorption coefficient at 1.25more » eV and a red-shifting of the optical absorption edge with increasing Sr fraction. The absorption spectra can be similarly tuned through the introduction of oxygen vacancies, indicating the critical role that nominal Fe valence plays in optical absorption. Dynamic optoelectronic properties were studied with ultrafast transient reflectance spectroscopy, revealing similar nanosecond photoexcited carrier lifetimes for oxygen deficient and stoichiometric films with the same nominal Fe valence. Furthermore, these results demonstrate that while the static optical absorption is strongly dependent on nominal Fe valence tuned through cation or anion stoichiometry, oxygen vacancies do not appear to play a significantly detrimental role in the recombination kinetics.« less

Direct-write maskless lithography using patterned oxidation of Si-substrate Induced by femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Kiani, Amirkianoosh; Venkatakrishnan, Krishnan; Tan, Bo

2013-03-01

In this study we report a new method for direct-write maskless lithography using oxidized silicon layer induced by high repetition (MHz) ultrafast (femtosecond) laser pulses under ambient condition. The induced thin layer of predetermined pattern can act as an etch stop during etching process in alkaline etchants such as KOH. The proposed method can be leading to promising solutions for direct-write maskless lithography technique since the proposed method offers a higher degree of flexibility and reduced time and cost of fabrication which makes it particularly appropriate for rapid prototyping and custom scale manufacturing. A Scanning Electron Microscope (SEM), Micro-Raman, Energy Dispersive X-ray (EDX), optical microscope and X-ray diffraction spectroscopy (XRD) were used to evaluate the quality of oxidized layer induced by laser pulses.

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 .

Dispersion-free continuum two-dimensional electronic spectrometer

PubMed Central

Zheng, Haibin; Caram, Justin R.; Dahlberg, Peter D.; Rolczynski, Brian S.; Viswanathan, Subha; Dolzhnikov, Dmitriy S.; Khadivi, Amir; Talapin, Dmitri V.; Engel, Gregory S.

2015-01-01

Electronic dynamics span broad energy scales with ultrafast time constants in the condensed phase. Two-dimensional (2D) electronic spectroscopy permits the study of these dynamics with simultaneous resolution in both frequency and time. In practice, this technique is sensitive to changes in nonlinear dispersion in the laser pulses as time delays are varied during the experiment. We have developed a 2D spectrometer that uses broadband continuum generated in argon as the light source. Using this visible light in phase-sensitive optical experiments presents new challenges in implementation. We demonstrate all-reflective interferometric delays using angled stages. Upon selecting an ~180 nm window of the available bandwidth at ~10 fs compression, we probe the nonlinear response of broadly absorbing CdSe quantum dots and electronic transitions of Chlorophyll a. PMID:24663470

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

NASA Astrophysics Data System (ADS)

Garnett, Joy Carleen

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

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

PubMed Central

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

2016-01-01

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

Ultrafast photoinduced charge separation in metal-semiconductor nanohybrids.

PubMed

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

2012-08-28

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

Experience-Related Structural Changes of Degenerated Occipital White Matter in Late-Blind Humans – A Diffusion Tensor Imaging Study

PubMed Central

Dietrich, Susanne; Hertrich, Ingo; Kumar, Vinod; Ackermann, Hermann

2015-01-01

Late-blind humans can learn to understand speech at ultra-fast syllable rates (ca. 20 syllables/s), a capability associated with hemodynamic activation of the central-visual system. Thus, the observed functional cross-modal recruitment of occipital cortex might facilitate ultra-fast speech processing in these individuals. To further elucidate the structural prerequisites of this skill, diffusion tensor imaging (DTI) was conducted in late-blind subjects differing in their capability of understanding ultra-fast speech. Fractional anisotropy (FA) was determined as a quantitative measure of the directionality of water diffusion, indicating fiber tract characteristics that might be influenced by blindness as well as the acquired perceptual skills. Analysis of the diffusion images revealed reduced FA in late-blind individuals relative to sighted controls at the level of the optic radiations at either side and the right-hemisphere dorsal thalamus (pulvinar). Moreover, late-blind subjects showed significant positive correlations between FA and the capacity of ultra-fast speech comprehension within right-hemisphere optic radiation and thalamus. Thus, experience-related structural alterations occurred in late-blind individuals within visual pathways that, presumably, are linked to higher order frontal language areas. PMID:25830371

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

NASA Astrophysics Data System (ADS)

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

2012-02-01

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

Plasmonic antennas as design elements for coherent ultrafast nanophotonics.

PubMed

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

2013-11-12

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

Probing ultrafast proton induced dynamics in transparent dielectrics

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

Development of integrated photonic-dicers for reformatting the point-spread-function of a telescope

NASA Astrophysics Data System (ADS)

MacLachlan, David G.; Harris, Robert; Choudhury, Debaditya; Arriola, Alexander; Brown, Graeme; Allington-Smith, Jeremy; Thomson, Robert R.

2014-07-01

Spectroscopy is a technique of paramount importance to astronomy, as it enables the chemical composition, distances and velocities of celestial objects to be determined. As the diameter of a ground-based telescope increases, the pointspread- function (PSF) becomes increasingly degraded due to atmospheric seeing. A degraded PSF requires a larger spectrograph slit-width for efficient coupling and current spectrographs for large telescopes are already on the metre scale. This presents numerous issues in terms of manufacturability, cost and stability. As proposed in 2010 by Bland-Hawthorn et al, one approach which may help to improve spectrograph stability is a guided wave transition, known as a "photonic-lantern". These devices enable the low-loss reformatting of a multimode PSF into a diffraction-limited source (in one direction). This pseudo-slit can then be used as the input to a traditional spectrograph operating at the diffraction limit. In essence, this approach may enable the use of diffractionlimited spectrographs on large telescopes without an unacceptable reduction in throughput. We have recently demonstrated that ultrafast laser inscription can be used to realize "integrated" photoniclanterns, by directly writing three-dimensional optical waveguide structures inside a glass substrate. This paper presents our work on developing ultrafast laser inscribed devices capable of reformatting a multimode telescope PSF into a diffraction-limited slit.

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.

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

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

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

2014-07-07

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

An ultrafast angle-resolved photoemission apparatus for measuring complex materials

NASA Astrophysics Data System (ADS)

Smallwood, Christopher L.; Jozwiak, Christopher; Zhang, Wentao; Lanzara, Alessandra

2012-12-01

We present technical specifications for a high resolution time- and angle-resolved photoemission spectroscopy setup based on a hemispherical electron analyzer and cavity-dumped solid state Ti:sapphire laser used to generate pump and probe beams, respectively, at 1.48 and 5.93 eV. The pulse repetition rate can be tuned from 209 Hz to 54.3 MHz. Under typical operating settings the system has an overall energy resolution of 23 meV, an overall momentum resolution of 0.003 Å-1, and an overall time resolution of 310 fs. We illustrate the system capabilities with representative data on the cuprate superconductor Bi2Sr2CaCu2O8+δ. The descriptions and analyses presented here will inform new developments in ultrafast electron spectroscopy.

Primary photochemical processes for Pt(iv) diazido complexes prospective in photodynamic therapy of tumors.

PubMed

Shushakov, Anton A; Pozdnyakov, Ivan P; Grivin, Vjacheslav P; Plyusnin, Victor F; Vasilchenko, Danila B; Zadesenets, Andrei V; Melnikov, Alexei A; Chekalin, Sergey V; Glebov, Evgeni M

2017-07-25

Diazide diamino complexes of Pt(iv) are considered as prospective prodrugs in oxygen-free photodynamic therapy (PDT). Primary photophysical and photochemical processes for cis,trans,cis-[Pt(N 3 ) 2 (OH) 2 (NH 3 ) 2 ] and trans,trans,trans-[Pt(N 3 ) 2 (OH) 2 (NH 3 ) 2 ] complexes were studied by means of stationary photolysis, nanosecond laser flash photolysis and ultrafast kinetic spectroscopy. The process of photolysis is multistage. The first stage is the photosubstitution of an azide ligand to a water molecule. This process was shown to be a chain reaction involving redox stages. Pt(iv) and Pt(iii) intermediates responsible for the chain propagation were recorded using ultrafast kinetic spectroscopy and nanosecond laser flash photolysis. The mechanism of photosubstitution is proposed.

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

PubMed

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

2017-04-18

Protons are vastly abundant in a wide range of exciting macromolecules and thus can be a powerful probe to investigate the structure and dynamics at atomic resolution using solid-state NMR (ssNMR) spectroscopy. Unfortunately, the high signal sensitivity, afforded by the high natural-abundance and high gyromagnetic ratio of protons, is greatly compromised by severe line broadening due to the very strong 1 H- 1 H dipolar couplings. As a result, protons are rarely used, in spite of the desperate need for enhancing the sensitivity of ssNMR to study a variety of systems that are not amenable for high resolution investigation using other techniques including X-ray crystallography, cryo-electron microscopy, and solution NMR spectroscopy. Thanks to the remarkable improvement in proton spectral resolution afforded by the significant advances in magic-angle-spinning (MAS) probe technology, 1 H ssNMR spectroscopy has recently attracted considerable attention in the structural and dynamics studies of various molecular systems. However, it still remains a challenge to obtain narrow 1 H spectral lines, especially from proteins, without resorting to deuteration. In this Account, we review recent proton-based ssNMR strategies that have been developed in our laboratory to further improve proton spectral resolution without resorting to chemical deuteration for the purposes of gaining atomistic-level insights into molecular structures of various crystalline solid systems, using small molecules and peptides as illustrative examples. The proton spectral resolution enhancement afforded by the ultrafast MAS frequencies up to 120 kHz is initially discussed, followed by a description of an ensemble of multidimensional NMR pulse sequences, all based on proton detection, that have been developed to obtain in-depth information from dipolar couplings and chemical shift anisotropy (CSA). Simple single channel multidimensional proton NMR experiments could be performed to probe the proximity of protons for structure determination using 1 H- 1 H dipolar couplings and to evaluate the changes in chemical environments as well as the relative orientation to the external magnetic field using proton CSA. Due to the boost in signal sensitivity enabled by proton detection under ultrafast MAS, by virtue of high proton natural abundance and gyromagnetic ratio, proton-detected multidimensional experiments involving low-γ nuclei can now be accomplished within a reasonable time, while the higher dimension also offers additional resolution enhancement. In addition, the application of proton-based ssNMR spectroscopy under ultrafast MAS in various challenging and crystalline systems is also presented. Finally, we briefly discuss the limitations and challenges pertaining to proton-based ssNMR spectroscopy under ultrafast MAS conditions, such as the presence of high-order dipolar couplings, friction-induced sample heating, and limited sample volume. Although there are still a number of challenges that must be circumvented by further developments in radio frequency pulse sequences, MAS probe technology and approaches to prepare NMR-friendly samples, proton-based ssNMR has already gained much popularity in various research domains, especially in proteins where uniform or site-selective deuteration can be relatively easily achieved. In addition, implementation of the recently developed fast data acquisition approaches would also enable further developments in the design and applications of proton-based ultrafast MAS multidimensional ssNMR techniques.

Ultrafast Fluorescence Spectroscopy via Upconversion: Applications to Biophysics

PubMed Central

Xu, Jianhua; Knutson, Jay R.

2012-01-01

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

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

LaRue, Jerry; Krejci, Ondrej; Yu, Liang

Here, the direct elucidation of the reaction pathways in heterogeneous catalysis has been challenging due the short-lived nature of reaction intermediates. Here, we directly measured on ultrafast timescales the initial hydrogenation steps of adsorbed CO on a Ru catalyst surface, which is known as the bottleneck reaction in syngas and CO 2 reforming processes. We initiated the hydrogenation of CO with an ultrafast laser temperature jump and probed transient changes in the electronic structure using real-time x-ray spectroscopy. In combination with theoretical simulations, we verified the formation of CHO during CO hydrogenation.

Initial Atomic Motion Immediately Following Femtosecond-Laser Excitation in Phase-Change Materials.

PubMed

Matsubara, E; Okada, S; Ichitsubo, T; Kawaguchi, T; Hirata, A; Guan, P F; Tokuda, K; Tanimura, K; Matsunaga, T; Chen, M W; Yamada, N

2016-09-23

Despite the fact that phase-change materials are widely used for data storage, no consensus exists on the unique mechanism of their ultrafast phase change and its accompanied large and rapid optical change. By using the pump-probe observation method combining a femtosecond optical laser and an x-ray free-electron laser, we substantiate experimentally that, in both GeTe and Ge_{2}Sb_{2}Te_{5} crystals, rattling motion of mainly Ge atoms takes place with keeping the off-center position just after femtosecond-optical-laser irradiation, which eventually leads to a higher symmetry or disordered state. This very initial rattling motion in the undistorted lattice can be related to instantaneous optical change due to the loss of resonant bonding that characterizes GeTe-based phase change materials. Based on the amorphous structure derived by first-principles molecular dynamics simulation, we infer a plausible ultrafast amorphization mechanism via nonmelting.

Revealing the nature of morphological changes in carbon nanotube-polymer saturable absorber under high-power laser irradiation.

PubMed

Chernysheva, Maria; Araimi, Mohammed Al; Rance, Graham A; Weston, Nicola J; Shi, Baogui; Saied, Sayah; Sullivan, John L; Marsh, Nicholas; Rozhin, Aleksey

2018-05-10

Composites of single-walled carbon nanotubes (SWNTs) and water-soluble polymers (WSP) are the focus of significant worldwide research due to a number of applications in biotechnology and photonics, particularly for ultrashort pulse generation. Despite the unique possibility of constructing non-linear optical SWNT-WSP composites with controlled optical properties, their thermal degradation threshold and limit of operational power remain unexplored. In this study, we discover the nature of the SWNT-polyvinyl alcohol (PVA) film thermal degradation and evaluate the modification of the composite properties under continuous high-power ultrashort pulse laser operation. Using high-precision optical microscopy and micro-Raman spectroscopy, we have examined SWNT-PVA films before and after continuous laser radiation exposure (up to 40 hours) with a maximum optical fluence of 2.3 mJ·cm -2 . We demonstrate that high-intensity laser radiation results in measurable changes in the composition and morphology of the SWNT-PVA film due to efficient heat transfer from SWNTs to the polymer matrix. The saturable absorber modification does not affect the laser operational performance. We anticipate our work to be a starting point for more sophisticated research aimed at the enhancement of SWNT-PVA films fabrication for their operation as reliable saturable absorbers in high-power ultrafast lasers.

Direct observation of multistep energy transfer in LHCII with fifth-order 3D electronic spectroscopy.

PubMed

Zhang, Zhengyang; Lambrev, Petar H; Wells, Kym L; Garab, Győző; Tan, Howe-Siang

2015-07-31

During photosynthesis, sunlight is efficiently captured by light-harvesting complexes, and the excitation energy is then funneled towards the reaction centre. These photosynthetic excitation energy transfer (EET) pathways are complex and proceed in a multistep fashion. Ultrafast two-dimensional electronic spectroscopy (2DES) is an important tool to study EET processes in photosynthetic complexes. However, the multistep EET processes can only be indirectly inferred by correlating different cross peaks from a series of 2DES spectra. Here we directly observe multistep EET processes in LHCII using ultrafast fifth-order three-dimensional electronic spectroscopy (3DES). We measure cross peaks in 3DES spectra of LHCII that directly indicate energy transfer from excitons in the chlorophyll b (Chl b) manifold to the low-energy level chlorophyll a (Chl a) via mid-level Chl a energy states. This new spectroscopic technique allows scientists to move a step towards mapping the complete complex EET processes in photosynthetic systems.

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

PubMed Central

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

2015-01-01

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

Spectroscopic Diagnosis of Excited-State Aromaticity: Capturing Electronic Structures and Conformations upon Aromaticity Reversal.

PubMed

Oh, Juwon; Sung, Young Mo; Hong, Yongseok; Kim, Dongho

2018-03-06

Aromaticity, the special energetic stability derived from cyclic [4 n + 2]π-conjugated electronic structures, has been the topic of intense interest in chemistry because it plays a critical role in rationalizing molecular stability, reactivity, and physical/chemical properties. Recently, the pioneering work by Colin Baird on aromaticity reversal, postulating that aromatic (antiaromatic) character in the ground state reverses to antiaromatic (aromatic) character in the lowest excited triplet state, has attracted much scientific attention. The completely reversed aromaticity in the excited state provides direct insight into understanding the photophysical/chemical properties of photoactive materials. In turn, the application of aromatic molecules to photoactive materials has led to numerous studies revealing this aromaticity reversal. However, most studies of excited-state aromaticity have been based on the theoretical point of view. The experimental evaluation of aromaticity in the excited state is still challenging and strenuous because the assessment of (anti)aromaticity with conventional magnetic, energetic, and geometric indices is difficult in the excited state, which practically restricts the extension and application of the concept of excited-state aromaticity. Time-resolved optical spectroscopies can provide a new and alternative avenue to evaluate excited-state aromaticity experimentally while observing changes in the molecular features in the excited states. Time-resolved optical spectroscopies take advantage of ultrafast laser pulses to achieve high time resolution, making them suitable for monitoring ultrafast changes in the excited states of molecular systems. This can provide valuable information for understanding the aromaticity reversal. This Account presents recent breakthroughs in the experimental assessment of excited-state aromaticity and the verification of aromaticity reversal with time-resolved optical spectroscopic measurements. To scrutinize this intriguing and challenging scientific issue, expanded porphyrins have been utilized as the ideal testing platform for investigating aromaticity because they show distinct aromatic and antiaromatic characters with aromaticity-specific spectroscopic features. Expanded porphyrins exhibit perfect aromatic and antiaromatic congener pairs having the same molecular framework but different numbers of π electrons, which facilitates the study of the pure effect of aromaticity by comparative analyses. On the basis of the characteristics of expanded porphyrins, time-resolved electronic and vibrational absorption spectroscopies capture the changes in electronic structure and molecular conformations driven by the change in aromaticity and provide clear evidence for aromaticity reversal in the excited states. The approaches described in this Account pave the way for the development of new and alternative experimental indices for the evaluation of excited-state aromaticity, which will enable overarching and fundamental comprehension of the role of (anti)aromaticity in the stability, dynamics, and reactivity in the excited states with possible implications for practical applications.

New styryl phenanthroline derivatives as model D-π-A-π-D materials for non-linear optics.

PubMed

Bonaccorso, Carmela; Cesaretti, Alessio; Elisei, Fausto; Mencaroni, Letizia; Spalletti, Anna; Fortuna, Cosimo Gianluca

2018-04-27

Four novel push-pull systems combining a central phenanthroline acceptor moiety and two substituted benzene rings, as a part of the conjugated π-system between the donor and the acceptor moieties, have been synthetized through a straightforward and efficient one-step synthetic procedure. The chromophores display high fluorescence and a peculiar fluorosolvatochromic behavior. Ultrafast investigation by means of state-of-the-art femtosecond-resolved transient absorption and fluorescence up-conversion spectroscopies allowed the role of intramolecular charge transfer (ICT) states to be evidenced, also revealing the crucial role played by both the polarity and proticity of the medium on the excited state dynamics of the chromophores. The ICT processes, responsible for the solvatochromism, also lead to interesting non-linear optical (NLO) properties: namely great two photon absorption cross-sections (hundreds of GM), investigated by the Two Photon Excited Fluorescence (TPEF) technique, and large second order hyperpolarizability coefficients, estimated through a convenient solvatochromic method. These features thus make the investigated styryl phenanthroline molecules model D-π-A-π-D compounds for non-linear optical applications. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hybrid photonic-crystal fiber

NASA Astrophysics Data System (ADS)

Markos, Christos; Travers, John C.; Abdolvand, Amir; Eggleton, Benjamin J.; Bang, Ole

2017-10-01

This article offers an extensive survey of results obtained using hybrid photonic-crystal fibers (PCFs) which constitute one of the most active research fields in contemporary fiber optics. The ability to integrate novel and functional materials in solid- and hollow-core PCFs through various postprocessing methods has enabled new directions toward understanding fundamental linear and nonlinear phenomena as well as novel application aspects, within the fields of optoelectronics, material and laser science, remote sensing, and spectroscopy. Here the recent progress in the field of hybrid PCFs is reviewed from scientific and technological perspectives, focusing on how different fluids, solids, and gases can significantly extend the functionality of PCFs. The first part of this review discusses the efforts to develop tunable linear and nonlinear fiber-optic devices using PCFs infiltrated with various liquids, glasses, semiconductors, and metals. The second part concentrates on recent and state-of-the-art advances in the field of gas-filled hollow-core PCFs. Extreme ultrafast gas-based nonlinear optics toward light generation in the extreme wavelength regions of vacuum ultraviolet, pulse propagation, and compression dynamics in both atomic and molecular gases, and novel soliton-plasma interactions are reviewed. A discussion of future prospects and directions is also included.

Growth, Faraday and inverse Faraday characteristics of Tb₂Ti₂O₇ crystal.

PubMed

Guo, Feiyun; Sun, Yilin; Yang, Xiongsheng; Chen, Xin; Zhao, Bin; Zhuang, Naifeng; Chen, Jianzhong

2016-03-21

Tb₂Ti₂O₇ (TTO) single crystal with dimensions of 20 × 20 × 16 mm³ was grown by the Czochralski method. Rietveld structure refinement of X-ray diffraction (XRD) data confirms that the compound crystallizes in the cubic system with pyrochlore structure. Transmission spectra, Magnetic circular dichroism (MCD) spectra, Faraday and inverse Faraday characteristics of TTO crystal have been measured and analyzed in detail. The results demonstrate that TTO crystal has high transmittance at 700-1400 nm waveband and a larger Verdat constant than that of TGG reported. Magnetic circular dichroism (MCD) spectra showed that the 4f→4f transitions of Tb³⁺ have significant contributions to the magneto-optical activity (MOA). In the time-resolved pump-probe spectroscopy, the rotation signals of the probe beam based on the inverse Faraday effect in magneto-optical crystal were observed at zero time delay, the full width at half maximum of the rotation and ellipticity signals can be as fast as ~500 fs, which indicates that TTO crystal can be a promising material for ultrafast all-optical magnetic switching.

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

DOE PAGES

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

2017-06-06

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

Exciton Relaxation and Electron Transfer Dynamics of Semiconductor Quantum Dots

NASA Astrophysics Data System (ADS)

Liu, Cunming

Quantum dots (QDs), also referred to as colloidal semiconductor nanocrystals, exhibit unique electronic and optical properties arising from their three-dimensional confinement and strongly enhanced coulomb interactions. Developing a detailed understanding of the exciton relaxation dynamics within QDs is important not only for sake of exploring the fundamental physics of quantum confinement processes, but also for their applications. Ultrafast transient absorption (TA) spectroscopy, as a powerful tool to explore the relaxation dynamics of excitons, was employed to characterize the hot single/multiexciton relaxation dynamics at the first four exciton states of CdSe/CdZnS QDs. We observed for the first time that the hot hole can relax through two possible pathways: Intraband multiple phonon coupling and intrinsic defect trapping, with a lifetime of ˜7 ps. Additionally, an ultra-short component of ˜ 8 ps, directly associated with the Auger recombination of highly energetic exciton states, was discovered. After exploring the exciton relaxation inside QDs, ultrafast TA spectroscopy was further applied to study the electron transferring outside from QDs. By using a brand-new photocatalytic system consisting of CdSe QDs and Ni-dihydrolipoic acid (Ni-DHLA) catalyst, which has represented a robust photocatalysis of H2 from water, the photoinduced electron transfer (ET) dynamics between QD and the catalyst, one of most important steps during H2 generation, was studied. We found smaller bare CdSe QDs exhibit a better ET performance and CdS shelling on the bare QDs leads to worsen the ET. The calculations of effective mass approximation (EMA) and Marcus theory show the ET process is mainly dominated by driving force, electronic coupling strength and reorganization energy between QD and the catalyst.

Ultrafast photo-initiated molecular quantum dynamics in the DNA dinucleotide d(ApG) revealed by broadband transient absorption spectroscopy.

PubMed

Stuhldreier, Mayra C; Temps, Friedrich

2013-01-01

The ultrafast photo-initiated quantum dynamics of the adenine-guanine dinucleotide d(ApG) in aqueous solution (pH 7) has been studied by femtosecond time-resolved spectroscopy after excitation at lambda = 260 nm. The results reveal a hierarchy of processes on time scales from tau < 100 fs to tau > 100 ps. Characteristic spectro-temporal signatures are observed indicating the transformation of the molecules in the electronic relaxation from the photo-excited state to a long-lived exciplex. In particular, broadband UV/VIS excited-state absorption (ESA) measurements detected a distinctive absorption by the excited dinucleotide around lambda = 335 nm, approximately 0.5 eV to the blue compared to the maximum of the broad and unstructured ESA spectrum after excitation of an equimolar mixture of the mononucleotides dAMP and dGMP. A similar feature has been identified as signature of the excimer in the dynamics of the adenine dinucleotide d(ApA). The lifetime of the d(ApG) exciplex was found to be tau = 124 +/- 4 ps both from the ESA decay time and from the ground-state recovery time, far longer than the sub-picosecond lifetimes of excited dAMP or dGMP. Fluorescence-time profiles measured by the up-conversion technique indicate that the exciplex state is reached around approximately 6 ps after excitation. Very weak residual fluorescence at longer times red-shifted to the emission from the photo-excited state shows that the exciplex is almost optically dark, but still has enough oscillator strength to give rise to the dual fluorescence of the dinucleotide in the static fluorescence spectrum.

Developing a structure-function model for the cryptophyte phycoerythrin 545 using ultrahigh resolution crystallography and ultrafast laser spectroscopy.

PubMed

Doust, Alexander B; Marai, Christopher N J; Harrop, Stephen J; Wilk, Krystyna E; Curmi, Paul M G; Scholes, Gregory D

2004-11-12

Cryptophyte algae differ from cyanobacteria and red algae in the architecture of their photosynthetic light harvesting systems, even though all three are evolutionarily related. Central to cryptophyte light harvesting is the soluble antenna protein phycoerythrin 545 (PE545). The ultrahigh resolution crystal structure of PE545, isolated from a unicellular cryptophyte Rhodomonas CS24, is reported at both 1.1A and 0.97A resolution, revealing details of the conformation and environments of the chromophores. Absorption, emission and polarized steady state spectroscopy (298K, 77K), as well as ultrafast (20fs time resolution) measurements of population dynamics are reported. Coupled with complementary quantum chemical calculations of electronic transitions of the bilins, these enable assignment of spectral absorption characteristics to each chromophore in the structure. Spectral differences between the tetrapyrrole pigments due to chemical differences between bilins, as well as their binding and interaction with the local protein environment are described. Based on these assignments, and considering customized optical properties such as strong coupling, a model for light harvesting by PE545 is developed which explains the fast, directional harvesting of excitation energy. The excitation energy is funnelled from four peripheral pigments (beta158,beta82) into a central chromophore dimer (beta50/beta61) in approximately 1ps. Those chromophores, in turn, transfer the excitation energy to the red absorbing molecules located at the periphery of the complex in approximately 4ps. A final resonance energy transfer step sensitizes just one of the alpha19 bilins on a time scale of 22ps. Furthermore, it is concluded that binding of PE545 to the thylakoid membrane is not essential for efficient energy transfer to the integral membrane chlorophyll a-containing complexes associated with PS-II.

What Controls the Rate of Ultrafast Charge Transfer and Charge Separation Efficiency in Organic Photovoltaic Blends.

PubMed

Jakowetz, Andreas C; Böhm, Marcus L; Zhang, Jiangbin; Sadhanala, Aditya; Huettner, Sven; Bakulin, Artem A; Rao, Akshay; Friend, Richard H

2016-09-14

In solar energy harvesting devices based on molecular semiconductors, such as organic photovoltaics (OPVs) and artificial photosynthetic systems, Frenkel excitons must be dissociated via charge transfer at heterojunctions to yield free charges. What controls the rate and efficiency of charge transfer and charge separation is an important question, as it determines the overall power conversion efficiency (PCE) of these systems. In bulk heterojunctions between polymer donor and fullerene acceptors, which provide a model system to understand the fundamental dynamics of electron transfer in molecular systems, it has been established that the first step of photoinduced electron transfer can be fast, of order 100 fs. But here we report the first study which correlates differences in the electron transfer rate with electronic structure and morphology, achieved with sub-20 fs time resolution pump-probe spectroscopy. We vary both the fullerene substitution and donor/fullerene ratio which allow us to control both aggregate size and the energetic driving force for charge transfer. We observe a range of electron transfer times from polymer to fullerene, from 240 fs to as short as 37 fs. Using ultrafast electro-optical pump-push-photocurrent spectroscopy, we find the yield of free versus bound charges to be weakly dependent on the energetic driving force, but to be very strongly dependent on fullerene aggregate size and packing. Our results point toward the importance of state accessibility and charge delocalization and suggest that energetic offsets between donor and acceptor levels are not an important criterion for efficient charge generation. This provides design rules for next-generation materials to minimize losses related to driving energy and boost PCE.

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

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

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

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

Nanosystems in ultrafast and superstrong fields: attosecond phenomena (Conference Presentation)

NASA Astrophysics Data System (ADS)

Stockman, Mark I.

2017-02-01

We present our latest results for a new class of phenomena in condensed matter nanooptics when a strong optical field ˜1-3 V/Å changes a solid within optical cycle [1-8]. Such a pulse drives ampere-scale currents in dielectrics and adiabatically controls their properties, including optical absorption and reflection, extreme UV absorption, and generation of high harmonics [9] in a non-perturbative manner on a 100-as temporal scale. Applied to a metal, such a pulse causes an instantaneous and, potentially, reversible change from the metallic to semimetallic properties. We will also discuss our latest theoretical results on graphene that in a strong ultrashort pulse field exhibits unique behavior [10-12]. New phenomena are predicted for buckled two-dimensional solids, silicene and germanene [13]. These are fastest phenomena in optics unfolding within half period of light. They offer potential for petahertz-bandwidth signal processing, generation of high harmonics on a nanometer spatial scale, etc. References 1. M. Durach, A. Rusina, M. F. Kling, and M. I. Stockman, Metallization of Nanofilms in Strong Adiabatic Electric Fields, Phys. Rev. Lett. 105, 086803-1-4 (2010). 2. M. Durach, A. Rusina, M. F. Kling, and M. I. Stockman, Predicted Ultrafast Dynamic Metallization of Dielectric Nanofilms by Strong Single-Cycle Optical Fields, Phys. Rev. Lett. 107, 086602-1-5 (2011). 3. A. Schiffrin, T. Paasch-Colberg, N. Karpowicz, V. Apalkov, D. Gerster, S. Muhlbrandt, M. Korbman, J. Reichert, M. Schultze, S. Holzner, J. V. Barth, R. Kienberger, R. Ernstorfer, V. S. Yakovlev, M. I. Stockman, and F. Krausz, Optical-Field-Induced Current in Dielectrics, Nature 493, 70-74 (2013). 4. M. Schultze, E. M. Bothschafter, A. Sommer, S. Holzner, W. Schweinberger, M. Fiess, M. Hofstetter, R. Kienberger, V. Apalkov, V. S. Yakovlev, M. I. Stockman, and F. Krausz, Controlling Dielectrics with the Electric Field of Light, Nature 493, 75-78 (2013). 5. V. Apalkov and M. I. Stockman, Metal Nanofilm in Strong Ultrafast Optical Fields, Phys. Rev. B 88, 245438-1-7 (2013). 6. V. Apalkov and M. I. Stockman, Theory of Dielectric Nanofilms in Strong Ultrafast Optical Fields, Phys. Rev. B 86, 165118-1-13 (2012). 7. F. Krausz and M. I. Stockman, Attosecond Metrology: From Electron Capture to Future Signal Processing, Nat. Phot. 8, 205-213 (2014). 8. O. Kwon, T. Paasch-Colberg, V. Apalkov, B.-K. Kim, J.-J. Kim, M. I. Stockman, and D. E. Kim, Semimetallization of Dielectrics in Strong Optical Fields, Sci. Rep, 6, 21272-1-9 (2016). 9. T. Higuchi, M. I. Stockman, and P. Hommelhoff, Strong-Field Perspective on High-Harmonic Radiation from Bulk Solids, Phys. Rev. Lett. 113, 213901-1-5 (2014). 10. H. K. Kelardeh, V. Apalkov, and M. I. Stockman, Wannier-Stark States of Graphene in Strong Electric Field, Phys. Rev. B 90, 085313-1-11 (2014). 11. H. K. Kelardeh, V. Apalkov, and M. I. Stockman, Graphene in Ultrafast and Superstrong Laser Fields, Phys. Rev. B 91, 0454391-8 (2015). 12. H. K. Kelardeh, V. Apalkov, and M. I. Stockman, Attosecond Strong-Field Interferometry in Graphene: Chirality, Singularity, and Berry Phase, Phys. Rev. B 93, 155434-1-7 (2016). 13. H. K. Kelardeh, V. Apalkov, and M. I. Stockman, Ultrafast Field Control of Symmetry, Reciprocity, and Reversibility in Buckled Graphene-Like Materials, Phys. Rev. B 92, 045413-1-9 (2015).

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

DOE PAGES

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

2017-08-15

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

Ultrafast Airy beam optical parametric oscillator

PubMed Central

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

2016-01-01

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

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

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

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

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

Time-resolved molecular imaging

NASA Astrophysics Data System (ADS)

Xu, Junliang; Blaga, Cosmin I.; Agostini, Pierre; DiMauro, Louis F.

2016-06-01

Time-resolved molecular imaging is a frontier of ultrafast optical science and physical chemistry. In this article, we review present and future key spectroscopic and microscopic techniques for ultrafast imaging of molecular dynamics and show their differences and connections. The advent of femtosecond lasers and free electron x-ray lasers bring us closer to this goal, which eventually will extend our knowledge about molecular dynamics to the attosecond time domain.

Ultrafast time-stretch imaging at 932 nm through a new highly-dispersive fiber

PubMed Central

Wei, Xiaoming; Kong, Cihang; Sy, Samuel; Ko, Ho; Tsia, Kevin K.; Wong, Kenneth K. Y.

2016-01-01

Optical glass fiber has played a key role in the development of modern optical communication and attracted the biotechnology researcher’s great attention because of its properties, such as the wide bandwidth, low attenuation and superior flexibility. For ultrafast optical imaging, particularly, it has been utilized to perform MHz time-stretch imaging with diffraction-limited resolutions, which is also known as serial time-encoded amplified microscopy (STEAM). Unfortunately, time-stretch imaging with dispersive fibers has so far mostly been demonstrated at the optical communication window of 1.5 μm due to lack of efficient dispersive optical fibers operating at the shorter wavelengths, particularly at the bio-favorable window, i.e., <1.0 μm. Through fiber-optic engineering, here we demonstrate a 7.6-MHz dual-color time-stretch optical imaging at bio-favorable wavelengths of 932 nm and 466 nm. The sensitivity at such a high speed is experimentally identified in a slow data-streaming manner. To the best of our knowledge, this is the first time that all-optical time-stretch imaging at ultrahigh speed, high sensitivity and high chirping rate (>1 ns/nm) has been demonstrated at a bio-favorable wavelength window through fiber-optic engineering. PMID:28018737

Ultrafast time-stretch imaging at 932 nm through a new highly-dispersive fiber.

PubMed

Wei, Xiaoming; Kong, Cihang; Sy, Samuel; Ko, Ho; Tsia, Kevin K; Wong, Kenneth K Y

2016-12-01

Optical glass fiber has played a key role in the development of modern optical communication and attracted the biotechnology researcher's great attention because of its properties, such as the wide bandwidth, low attenuation and superior flexibility. For ultrafast optical imaging, particularly, it has been utilized to perform MHz time-stretch imaging with diffraction-limited resolutions, which is also known as serial time-encoded amplified microscopy (STEAM). Unfortunately, time-stretch imaging with dispersive fibers has so far mostly been demonstrated at the optical communication window of 1.5 μm due to lack of efficient dispersive optical fibers operating at the shorter wavelengths, particularly at the bio-favorable window, i.e., <1.0 μm. Through fiber-optic engineering, here we demonstrate a 7.6-MHz dual-color time-stretch optical imaging at bio-favorable wavelengths of 932 nm and 466 nm. The sensitivity at such a high speed is experimentally identified in a slow data-streaming manner. To the best of our knowledge, this is the first time that all-optical time-stretch imaging at ultrahigh speed, high sensitivity and high chirping rate (>1 ns/nm) has been demonstrated at a bio-favorable wavelength window through fiber-optic engineering.

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

PubMed

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

2014-05-23

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

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

PubMed Central

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

2014-01-01

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

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

NASA Astrophysics Data System (ADS)

Amsden, Jason J.

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

Ultrafast terahertz spectroscopy study of a Kondo insulating thin-film Sm B6 : Evidence for an emergent surface state

NASA Astrophysics Data System (ADS)

Zhang, Jingdi; Yong, Jie; Takeuchi, Ichiro; Greene, Richard L.; Averitt, Richard D.

2018-04-01

We utilize terahertz time domain spectroscopy to investigate thin films of the heavy fermion compound Sm B6 , a prototype Kondo insulator. Temperature-dependent terahertz (THz) conductivity measurements reveal a rapid decrease in the Drude weight and carrier scattering rate at ˜T*=20 K , well below the hybridization gap onset temperature (100 K). Moreover, a low-temperature conductivity plateau (below 20 K) suggests the emergence of a surface state with an effective electron mass of 0.1 me . The conductivity dynamics following optical excitation is also measured and interpreted using Rothwarf-Taylor (R-T) phenomenology, yielding a hybridization gap energy of 17 meV. However, R-T modeling of the conductivity dynamics reveals a deviation from the expected thermally excited quasiparticle density at temperatures below 20 K, indicative of another channel opening up in the low-energy electrodynamics. Taken together, these results are consistent with the onset of a surface state well below the crossover temperature (100 K) after long-range coherence of the f -electron Kondo lattice is established.

Canadian Semiconductor Technology Conference, 6th, Ottawa, Canada, Aug. 11-13, 1992, Proceedings

NASA Astrophysics Data System (ADS)

Baribeau, Jean-Marc

1992-11-01

This volume contains papers on the growth efficiency and distribution coefficient of GaInP-InP epilayers and heterostructures, X-ray photoelectron spectroscopy studies of Ge epilayers on Si(100), and mechanical properties of silicon carbide films for X-ray lithography application. Attention is also given to fine structure in Raman spectroscopy and X-ray reflectometry and its uses for the characterization of superlattices, phase formation in Fe-Si thin-film diffusion couples, process optimization for a micromachined silicon nonreverse valve, and a numerical study of heat transport in thermally isolated flow-rate microsensors. Particular consideration is given to a versatile 2D model for InGaAsP quantum-well semiconductor lasers, gallium arsenide electronics in the marketplace, and optical channel grading in p-type Si/SiGe MOSFETs. Other papers are on ultrafast electron tunneling in a reverse-biased high-efficiency quantum well laser structure, excess currents as a result of trap-assisted tunneling in double-barrier resonant tunneling diodes, and carrier lifetimes in strained InGaAsP multiple quantum-well laser structures.

Strongly bound excitons in anatase TiO 2 single crystals and nanoparticles

DOE PAGES

Baldini, E.; Chiodo, L.; Dominguez, A.; ...

2017-04-13

Anatase TiO 2 is among the most studied materials for light-energy conversion applications, but the nature of its fundamental charge excitations is still unknown. Yet it is crucial to establish whether light absorption creates uncorrelated electron-hole pairs or bound excitons and, in the latter case, to determine their character. Here, by combining steady-state angle-resolved photoemission spectroscopy and spectroscopic ellipsometry with state-of-the-art ab initio calculations, we demonstrate that the direct optical gap of single crystals is dominated by a strongly bound exciton rising over the continuum of indirect interband transitions. This exciton possesses an intermediate character between the Wannier-Mott and Frenkelmore » regimes and displays a peculiar two-dimensional wavefunction in the three-dimensional lattice. The nature of the higher-energy excitations is also identified. Furthermore, the universal validity of our results is confirmed up to room temperature by observing the same elementary excitations in defect-rich samples (doped single crystals and nanoparticles) via ultrafast two-dimensional deep-ultraviolet spectroscopy.« less