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At least 19 records

Plasmon resonance enhanced large third-order optical nonlinearity and ultrafast optical response in Au nanobipyramids

The third-order optical nonlinearity and response time of Au nanobipyramids have been investigated by using optical Kerr effect technique. Large third-order nonlinear optical susceptibility (χ{sup (3)}) and ultrafast optical response time have been obtained at the longitudinal surface plasmon resonance (LSPR) wavelength. As the excitation laser wavelength varies from non-resonance wavelength of 780 nm to the LSPR wavelength of 825 nm, χ{sup (3)} increases from 7.4 × 10{sup −14} to 3.9 × 10{sup −13} esu, the fast component of the response time decreases from 141 ± 23 to 83 ± 8 fs and the ratio of the fast component remains around 48%, while the slow response time decreases from 3200 ± 200 to 2310 ± 158 fs. The large enhancement of χ{sup (3)} is due to the large local field enhancement caused by the surface plasmon resonance, and the shortening of the response times are induced by the increased probability of the electron-electron and electron-phonon scatterings in the nanosystem. This significant ultrafast optical property in Au nanobipyramids has great application in future ultrafast information processors.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

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

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.

47 OTHER INSTRUMENTATION↗

Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes

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.

36 MATERIALS SCIENCE↗

Ultrafast optical properties of lithographically defined quantum dot amplifiers

We measure the ultrafast optical response of lithographically defined quantum dot amplifiers at 40 K. Recovery of the gain mostly occurs in less than 1 picosecond, with some longer-term transients attributable to carrier heating. Recovery of the absorption proceeds on a much longer timescale, representative of relaxation between quantum dot levels and carrier recombination. We also measure transparency current-density in these devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

In-situ weak-beam and polarization control of multidimensional laser sidebands for ultrafast optical switching

All-optical switching has myriad applications in optoelectronics, optical communications, and quantum information technology. To achieve ultrafast optical switching in a compact yet versatile setup, we demonstrate distinct sets of two-dimensional (2D) broadband up-converted multicolor arrays (BUMAs) in a thin type-I β-barium-borate crystal with two noncollinear near-IR femtosecond pulses at various phase-matching conditions. The unique interaction mechanism is revealed as quadratic spatial solitons (QSSs)-coupled cascaded four-wave mixing (CFWM), corroborated by numerical calculations of the governing phase-matching conditions. Broad and continuous spectral-spatial tunability of the 2D BUMAs are achieved by varying the time delay between the two incident pulses that undergo CFWM interaction, rooted in the chirped nature of the weak white light and the QSSs generation of the intense fundamental beam. The control of 2D BUMAs is accomplished via seeding a weak second-harmonic pulse in situ to suppress the 2D arrays with polarization dependence on the femtosecond timescale that matches the control pulse duration of ∼35 fs. A potential application is proposed on femtosecond all-optical switching in an integrated wavelength-time division multiplexing device.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

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

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.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Ultrafast Optically Induced Perturbation of Oxygen Octahedral Rotations in Multiferroic BiFeO 3 Thin Films

The functional properties of complex oxides, including magnetism and ferroelectricity, are closely linked to subtle structural distortions. Ultrafast optical excitations provide the means to manipulate structural features and ultimately to affect the functional properties of complex oxides with picosecond-scale precision. Here, we report that the lattice expansion of multiferroic BiFeO 3 following above-bandgap optical excitation leads to distortion of the oxygen octahedral rotation (OOR) pattern. The continuous coupling between OOR and strain was probed using time-resolved X-ray free-electron laser diffraction with femtosecond time resolution. Density functional theory calculations predict a relationship between the OOR and the elastic strain consistent with the experiment, demonstrating a route to employing this approach in a wider range of systems. Ultrafast control of the functional properties of BiFeO 3 thin films is enabled by this approach because the OOR phenomena are related to ferroelectricity, and via the Fe-O-Fe bond angles, the superexchange interaction between Fe atoms.

36 MATERIALS SCIENCE↗

Energy Transfer from Antenna Ligand to Europium(III) Followed Using Ultrafast Optical and X-ray Spectroscopy

A series of highly luminescent europium(III) complexes which exhibit photoluminescence from the Eu(III) center following energy transfer from the UV absorbing organic sensitizer have been investigated using a combination of ultrafast optical transient absorption and Eu L3 X-ray transient absorption techniques. We have previously demon- strated that the latter can be used as a signature of 4f–4f excitation responsible for the photoluminescence in these Eu(III) coordination complexes, but the long time scale of the earlier measurements did not allow direct observation of the ligand-to-metal energy transfer step, preventing a determi- nation of the sensitization mechanism. Here, we provide the first direct experimental verification that Dexter electron exchange from the ligand triplet state is the dominant energy transfer mechanism in these photoluminescent systems. Moreover, the optical transient absorption results obtained herein imply that energy transfer for all three compounds has near unity yield, regardless of differences in the sensitization efficiencies, suggesting that the variations in the sensitization efficiencies are determined almost entirely by differences in the ligand-centered intersystem crossing rates. As a result, the implications for the rational design of more effective photoluminescent lanthanide complexes are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultrafast optical switches using quantum wells

Colloidal quantum wells have discrete energy states and electrons in the quantum wells undergo interband and intersubband state transitions. The transmissivity of a colloidal quantum well may be tuned by actively controlling the states of the colloidal quantum wells enabling ultrafast optical switching. A primary excitation source is configured to provide a primary excitation to promote a colloidal quantum well from a ground state to a first excitation state. A secondary excitation source is configured to provide a secondary excitation to the colloidal quantum well to promote the colloidal quantum well from the first excitation state to the second excitation state with the first and second excitation states being subbands in the conduction band of the colloidal quantum well.

Diroll, Benjamin↗

Spin-current-mediated rapid magnon localisation and coalescence after ultrafast optical pumping of ferrimagnetic alloys

Sub-picosecond magnetisation manipulation via femtosecond optical pumping has attracted wide attention ever since its original discovery in 1996. Furthermore, the spatial evolution of the magnetisation is not yet well understood, in part due to the difficulty in experimentally probing such rapid dynamics. Here, we find evidence of rapid magnetic order recovery in materials with perpendicular magnetic anisotropy via nonlinear magnon processes. We identify both localisation and coalescence regimes, whereby localised magnetic textures nucleate and subsequently evolve in accordance with a power law formalism. Coalescence is observed for optical excitations both above and below the switching threshold. Simulations indicate that the ultrafast generation of noncollinear magnetisation via optical pumping establishes exchange-mediated spin currents with an equivalent 100% spin polarised charge current density of 108 A/cm 2 . Such large spin currents precipitate rapid recovery of magnetic order after optical pumping. These processes suggest an ultrafast optical route for the stabilization of desired meta-stable states, e.g., isolated skyrmions.

36 MATERIALS SCIENCE↗

Spin-current-mediated rapid magnon localisation and coalescence after ultrafast optical pumping of ferrimagnetic alloys

We identify both localisation and coalescence regimes, whereby localised magnetic textures nucleate and subsequently evolve in accordance with a power law formalism. Coalescence is observed for optical excitations both above and below the switching threshold. Simulations indicate that the ultrafast generation of noncollinear magnetisation via optical pumping establishes exchange-mediated spin currents with an equivalent 100% spin polarised charge current density of 108 A/cm2. Such large spin currents precipitate rapid recovery of magnetic order after optical pumping. These processes suggest an ultrafast optical route for the stabilization of desired meta-stable states, e.g., isolated skyrmions.

14 SOLAR ENERGY↗

Ultrafast optical pump-probe spectroscopy is used to reveal the coexistence of coupled antiferromagnetic (AFM)/ferroelectric (FE) and ferromagnetic (FM) orders in multiferroic TbMnO3 films, which can guide researchers in creating new kinds of multiferroic materials.

Multiferroic materials have attracted much interest in the past decade, due not only to their novel device applications, but also their manifestations of coupling and interactions between different order parameters (particularly electric polarization and magnetic order). Recently, much attention has been focused on perovskite manganites, RMnO{sub 3} (R = rare earth ions), due to the discovery of a large magnetoelectric effect in these materials. The first member of this family to be discovered was TbMnO{sub 3} (TMO), which is now well established as a typical magnetoelectric multiferroic. Extensive experimental and theoretical studies have already been done on single crystal TMO (SC-TMO). In brief, SC-TMO, with a distorted orthorhombic perovskite structure, has an antiferromagnetic (AFM) phase transition at T{sub N} {approx}40 K with sinusoidally ordered Mn moments. Below T{sub FE} {approx} 28 K, ferroelectric (FE) order develops owing to the appearance of cycloidal spiral spin structure. In contrast, there are relatively few reports describing the properties of TMO thin films (typically grown on SrTiO{sub 3} (STO) substrates). In general, thin films can enable new functionality in materials, as their physical parameters can be changed by modifying their structure via strain imposed by the substrate. Strain in particular has the potential to directly couple FE and FM orders, which is very rare. This could benefit electronic device applications by providing low power consumption, high speed operation, and greater electric/magnetic field controllability. Previous investigations of magnetic properties in TMO films revealed an unexpected ferromagnetic (FM) order, in contrast to SC-TMO. However, several important questions regarding these films are still unanswered for instance: (1) What mechanism induces FM order? (2) Can FM, sinusoidal AFM and spiral AFM (or FE) orders coexist? (3) Can FM order be coupled to FE order? To fully understand these unique materials, experimental techniques capable of dynamically unraveling the interplay between these degrees of freedom on an ultrafast timescale are needed. Here, we use ultrafast optical pump-probe spectroscopy to reveal coexisting coupled magnetic orders in epitaxial TMO thin films grown on (001)-STO, which were not observed in previous work. Our temperature (T)-dependent transient differential reflectivity ({Delta}R/R) measurements show clear signatures of sinusoidal AFM, spiral AFM (FE) and FM phases developing as the film thickness changes. We carry out first-principle density functional theory (DFT) calculations to explain the coupling between AFM/FE and FM orders. These results reveal that the coupling between different magnetic orders observed in our multiferroic TMO thin films may offer greater control of functionality as compared to bulk single crystal multiferroics.

36 MATERIALS SCIENCE↗

Ultrafast optical control of magnetization dynamics in polycrystalline bismuth doped iron garnet thin films

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.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Is perpendicular magnetic anisotropy essential to all-optical ultrafast spin reversal in ferromagnets?

All-optical spin reversal presents a new opportunity for spin manipulations, free of a magnetic field. Most of all-optical-spin-reversal ferromagnets are found to have a perpendicular magnetic anisotropy (PMA), but it has been unknown whether PMA is necessary for spin reversal. Here we theoretically investigate magnetic thin films with either PMA or in-plane magnetic anisotropy (IMA). Our results show that spin reversal in IMA systems is possible, but only with a longer laser pulse and within a narrow laser parameter region. Spin reversal does not show a strong helicity dependence where the left- and right-circularly polarized light lead to the identical results. By contrast, the spin reversal in PMA systems is robust, provided both the spin angular momentum and laser field are strong enough while the magnetic anisotropy itself is not too strong. This explains why experimentally the majority of all-optical spin-reversal samples are found to have strong PMA and why spins in Fe nanoparticles only cant out of plane. It is the laser-induced spin–orbit torque that plays a key role in the spin reversal. Surprisingly, the same spin–orbit torque results in laser-induced spin rectification in spin-mixed configuration, a prediction that can be tested experimentally. Our results clearly point out that PMA is essential to spin reversal, though there is an opportunity for in-plane spin reversal.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Wavelet analysis of molecular dynamics: Efficient extraction of time-frequency information in ultrafast optical processes

New experimental techniques based on nonlinear ultrafast spectroscopies have been developed over the last few years, and have been demonstrated to provide powerful probes of quantum dynamics in different types of molecular aggregates, including both natural and artificial light harvesting complexes. Fourier transform-based spectroscopies have been particularly successful, yet “complete” spectral information normally necessitates the loss of all information on the temporal sequence of events in a signal. This information though is particularly important in transient or multi-stage processes, in which the spectral decomposition of the data evolves in time. By going through several examples of ultrafast quantum dynamics, we demonstrate that the use of wavelets provide an efficient and accurate way to simultaneously acquire both temporal and frequency information about a signal, and argue that this greatly aids the elucidation and interpretation of physical process responsible for non-stationary spectroscopic features, such as those encountered in coherent excitonic energy transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗