Chih-Wei Luo

Epitaxial Photostriction-Magnetostriction Coupled Self-Assembled Nanostructures

Self-assembled vertical nanostructures take advantage of high interface-to-volume ratio and can be used to design new functionalities by the choice of a proper combination of constituents. However, most of the studies to date have emphasized the functional controllability of the nanostructures using external electric or magnetic fields. In this study, to introduce light (or photons) as an external control parameter in a self-assembled nanostructure system, we have successfully synthesized oxide nanostructures with CoFe(2)O(4) nanopillars embedded in a SrRuO(3) matrix. The combination of photostrictive SrRuO(3) and magnetostrictive CoFe(2)O(4) in the intimately assembled nanostructures leads to a light-induced, ultrafast change in magnetization of the CoFe(2)O(4) nanopillars. Our work demonstrates a novel concept on oxide nanostructure design and opens an alternative pathway for the explorations of diverse functionalities in heteroepitaxial self-assembled oxide nanostructures.

Quasiparticle Dynamics and Phonon Softening in FeSe Superconductors

Quasiparticle dynamics of FeSe single crystals revealed by dual-color transient reflectivity measurements (ΔR/R) provides unprecedented information on Fe-based superconductors. The amplitude of the fast component in ΔR/R clearly gives a competing scenario between spin fluctuations and superconductivity. Together with the transport measurements, the relaxation time analysis further exhibits anomalous changes at 90 and 230 K. The former manifests a structure phase transition as well as the associated phonon softening. The latter suggests a previously overlooked phase transition or crossover in FeSe. The electron-phonon coupling constant λ is found to be 0.16, identical to the value of theoretical calculations. Such a small λ demonstrates an unconventional origin of superconductivity in FeSe.

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

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.

Ultrafast thermoelastic dynamics of HoMnO(3) single crystals derived from femtosecond optical pump-probe spectroscopy

In this paper, the photo-induced ultrafast thermoelastic dynamics of hexagonal HoMnO3 single crystals has been studied by using optical pump–probe spectroscopy. The thermoelastic effect in the ab-plane of hexagonal HoMnO3, associated with giant magnetoelastic coupling around the Neel temperature (TN), is intimately correlated to the emergence of a negative component in the transient reflectivity changes (ΔR/R) obtained in temperature-dependent pump–probe experiments. Moreover, the variation in the oscillation period in ΔR/R caused by a strain pulse propagating along the c-axis exhibits an abrupt drop around TN, presumably due to the antiferromagnetic-ordering-induced changes in ferroelectricity.

Synthesis and characterization of a highly two-photon active dendrimer derived from 2,3,8-trifunctionalized indenoquinoxaline units

A dendritic chromophore derived from 2,3,8-trifunctionalized indenoquinoxaline units was synthesized and experimentally shown to manifest very strong and widely-dispersed two-photon absorption (2PA) across the dynamic tuning range of a Ti:sapphire laser. The maximum 2PA of the studied chromophore was found to reach ≈31 700 GM, indicating that 2,3,8-trifuctionalized indenoquinoxaline units are useful building moieties for the construction of highly active 2PA-dyes. In addition, this dendritic structure was also demonstrated to effectively regulate the optical power of femtosecond laser pulses at 800 nm.

THz emission from organic cocrystalline salt: 2, 6-diaminopyridinium-4-nitrophenolate-4-nitrophenol

We report few-cycle THz pulses emission from a novel organic crystal 2,6-diaminopyridinium-4-nitrophenolate-4-nitrophenol (DAP+NP-NP). The observed amplitude of the THz electric field from a DAP+NP-NP crystal is comparable with that from a ZnTe single crystal under the same optical pumping conditions. Both the waveform and spectra of the THz radiation from DAP+NP-NP are similar to those from ZnTe. We conclude that a high quality DAP+NP-NP crystal would be a high potential candidate in THz generation and applications.

Use of Ultrafast Time-Resolved Spectroscopy to Demonstrate the Effect of Annealing on the Performance of P3HT:PCBM Solar Cells

The organic solar cells of heterojunction system, ITO/PEDOT:PSS/P3HT:PCBM/Al, with a thermal annealing after deposition of Al exhibit better performance than those with an annealing process before deposition of Al. In this study, ultrafast time-resolved spectroscopy is employed to reveal the underlying mechanism of annealing effects on the performance of P3HT:PCBM solar cell devices. The analyses of all decomposed relaxation processes show that the postannealed devices exhibit an increase in charge transfer, in the number of separated polarons and a reduction in the amount of recombination between excited carriers. Moreover, the longer lifetime for the excited carriers in postannealed devices indicates it is more likely to be dissociated into photocarriers and result in a larger value for photocurrent, which demonstrates the physical mechanism for increased device performance.

Environment-dependent ultrafast photoisomerization dynamics in azo dye.

Azoaromatic dyes have been extensively investigated over the past decade due to their potential use in a variety of optical devices that exploit their ultrafast photoisomerization processes. Among the azoaromatic dyes, Disperse Red 19 is a commercially available azobenzene nonlinear optical chromophore with a relatively high ground-state dipole moment. In the present study, we used ultrafast time-resolved spectroscopy to clarify the dynamics of a push-pull substituted azobenzene dye. Solution and film samples exhibited different ultrafast dynamics, indicating that the molecular environment affects the photoisomerization dynamics of the dye.

Superior local conductivity in self-organized nanodots on indium-tin-oxide films induced by femtosecond laser pulses

Large-area surface ripple structures of indium-tin-oxide films, composed of self-organized nanodots, were induced by femtosecond laser pulses, without scanning. The multi-periodic spacing (~800 nm, ~400 nm and ~200 nm) was observed in the laser-induced ripple of ITO films. The local conductivity of ITO films is significantly higher, by approximately 30 times, than that of the as-deposited ITO films, due to the formation of these nanodots. Such a significant change can be ascribed to the formation of indium metal-like clusters, which appear as budges of ~5 nm height, due to an effective volume increase after breaking the In-O to form In-In bonding.

Pulsed terahertz radiation due to coherent phonon-polariton excitation in 〈110〉 ZnTe crystal

Pulsed terahertz (THz) radiation, generated through optical rectification (OR) by exciting 〈110〉 ZnTe crystal with ultrafast optical pulses, typically consists of only a few-cycles of electromagnetic field oscillations with a duration about a couple of picoseconds. However, it is possible, under appropriate conditions, to generate a long damped oscillation tail (LDOT) following the main cycles. The LDOT can last tens of picoseconds and its Fourier transform shows a higher and narrower frequency peak than that of the main pulse. We have demonstrated that the generation of the LDOT depends on both the duration of the optical pulse and its central wavelength. Furthermore, we have also performed theoretical calculations based upon the OR effect coupled with the phonon-polariton mode of ZnTe and obtained theoretical THz waveforms in good agreement with our experimental observation.