Chan La-o-vorakiat

Ultrafast magnetization enhancement in metallic multilayers driven by superdiffusive spin current

Uncovering the physical mechanisms that govern ultrafast charge and spin dynamics is crucial for understanding correlated matter as well as the fundamental limits of ultrafast spin-based electronics. Spin dynamics in magnetic materials can be driven by ultrashort light pulses, resulting in a transient drop in magnetization within a few hundred femtoseconds. However, a full understanding of femtosecond spin dynamics remains elusive. Here we spatially separate the spin dynamics using Ni/Ru/Fe magnetic trilayers, where the Ni and Fe layers can be ferro- or antiferromagnetically coupled. By exciting the layers with a laser pulse and probing the magnetization response simultaneously but separately in Ni and Fe, we surprisingly find that optically induced demagnetization of the Ni layer transiently enhances the magnetization of the Fe layer when the two layer magnetizations are initially aligned parallel. Our observations are explained by a laser-generated superdiffusive spin current between the layers.

Probing the timescale of the exchange interaction in a ferromagnetic alloy

The underlying physics of all ferromagnetic behavior is the cooperative interaction between individual atomic magnetic moments that results in a macroscopic magnetization. In this work, we use extreme ultraviolet pulses from high-harmonic generation as an element-specific probe of ultrafast, optically driven, demagnetization in a ferromagnetic Fe-Ni alloy (permalloy). We show that for times shorter than the characteristic timescale for exchange coupling, the magnetization of Fe quenches more strongly than that of Ni. Then as the Fe moments start to randomize, the strong ferromagnetic exchange interaction induces further demagnetization in Ni, with a characteristic delay determined by the strength of the exchange interaction. We can further enhance this delay by lowering the exchange energy by diluting the permalloy with Cu. This measurement probes how the fundamental quantum mechanical exchange coupling between Fe and Ni in magnetic materials influences magnetic switching dynamics in ferromagnetic materials relevant to next-generation data storage technologies.

High numerical aperture tabletop soft x-ray diffraction microscopy with 70-nm resolution.

Light microscopy has greatly advanced our understanding of nature. The achievable resolution, however, is limited by optical wavelengths to ≈200 nm. By using imaging and labeling technologies, resolutions beyond the diffraction limit can be achieved for specialized specimens with techniques such as near-field scanning optical microscopy, stimulated emission depletion microscopy, and photoactivated localization microscopy. Here, we report a versatile soft x-ray diffraction microscope with 70- to 90-nm resolution by using two different tabletop coherent soft x-ray sources—a soft x-ray laser and a high-harmonic source. We also use field curvature correction that allows high numerical aperture imaging and near-diffraction-limited resolution of 1.5λ. A tabletop soft x-ray diffraction microscope should find broad applications in biology, nanoscience, and materials science because of its simple optical design, high resolution, large depth of field, 3D imaging capability, scalability to shorter wavelengths, and ultrafast temporal resolution.

Elucidating the role of disorder and free-carrier recombination kinetics in CH3NH3PbI3 perovskite films.

Apart from broadband absorption of solar radiation, the performance of photovoltaic devices is governed by the density and mobility of photogenerated charge carriers. The latter parameters indicate how many free carriers move away from their origin, and how fast, before loss mechanisms such as carrier recombination occur. However, only lower bounds of these parameters are usually obtained. Here we independently determine both density and mobility of charge carriers in a perovskite film by the use of time-resolved terahertz spectroscopy. Our data reveal the modification of the free carrier response by strong backscattering expected from these heavily disordered perovskite films. The results for different phases and different temperatures show a change of kinetics from two-body recombination at room temperature to three-body recombination at low temperatures. Our results suggest that perovskite-based solar cells can perform well even at low temperatures as long as the three-body recombination has not become predominant.

Tabletop soft-x-ray Fourier transform holography with 50 nm resolution

We present what we believe to be the first implementation of Fourier transform (FT) holography using a tabletop coherent x-ray source. By applying curvature correction to compensate for the large angles inherent in high-NA coherent imaging, we achieve image resolution of 89 nm using high-harmonic beams at a wavelength of 29 nm. Moreover, by combining holography with iterative phase retrieval, we improve the image resolution to <53 nm. We also demonstrate that FT holography can be used effectively with short exposure times of 30 s. This technique will enable biological and materials microscopy with simultaneously high spatial and temporal resolution on a tabletop soft-x-ray source.

Graphene Terahertz Modulators by Ionic Liquid Gating

Graphene based THz modulators are promising due to the conical band structure and high carrier mobility of graphene. Here, we tune the Fermi level of graphene via electrical gating with the help of ionic liquid to control the THz transmittance. It is found that, in the THz range, both the absorbance and reflectance of the device increase proportionately to the available density of states due to intraband transitions. Compact, stable, and repeatable THz transmittance modulation up to 93% (or 99%) for a single (or stacked) device has been demonstrated in a broad frequency range from 0.1 to 2.5 THz, with an applied voltage of only 3 V at room temperature.

Terahertz Conductivity of Twisted Bilayer Graphene

Using terahertz time-domain spectroscopy, the real part of optical conductivity [σ(1)(ω)] of twisted bilayer graphene was obtained at different temperatures (10-300 K) in the frequency range 0.3-3 THz. On top of a Drude-like response, we see a strong peak in σ(1)(ω) at ~2.7 THz. We analyze the overall Drude-like response using a disorder-dependent (unitary scattering) model, then attribute the peak at 2.7 THz to an enhanced density of states at that energy, which is caused by the presence of a van Hove singularity arising from a commensurate twisting of the two graphene layers.

Phonon Mode Transformation Across the Orthohombic–Tetragonal Phase Transition in a Lead Iodide Perovskite CH3NH3PbI3: A Terahertz Time-Domain Spectroscopy Approach

We study the temperature-dependent phonon modes of the organometallic lead iodide perovskite CH3NH3PbI3 thin film across the terahertz (0.5-3 THz) and temperature (20-300 K) ranges. These modes are related to the vibration of the Pb-I bonds. We found that two phonon modes in the tetragonal phase at room temperature split into four modes in the low-temperature orthorhombic phase. By use of the Lorentz model fitting, we analyze the critical behavior of this phase transition. The carrier mobility values calculated from the low-temperature phonon mode frequencies, via two theoretical approaches, are found to agree reasonably with the experimental value (∼2000 cm(2) V(-1) s(-1)) from a previous time-resolved THz spectroscopy work. Thus, we have established a possible link between terahertz phonon modes and the transport properties of perovskite-based solar cells.

Optical properties of organometallic perovskite: An ab initio study using relativistic GW correction and Bethe-Salpeter equation

In the development of highly efficient photovoltaic cells, solid perovskite systems have demonstrated unprecedented promise, with the figure of merit exceeding nineteen percent of efficiency. In this paper, we investigate the optical and vibrational properties of organometallic cubic perovskite CH3NH3PbI3 using first-principles calculations. For accurate theoretical description, we go beyond conventional density functional theory (DFT), and calculated optical conductivity using relativist quasi-particle (GW) correction. Incorporating these many-body effects, we further solve Bethe-Salpeter equations (BSE) for excitons, and found enhanced optical conductivity near the gap edge. Due to the presence of organic methylammonium cations near the center of the perovskite cell, the system is sensitive to low energy vibrational modes. We estimate the phonon modes of CH3NH3PbI3 using small displacement approach, and further calculate the infrared absorption (IR) spectra. Qualitatively, our calculations of low-energy phonon frequencies are in good agreement with our terahertz measurements. Therefore, for both energy scales (around 2 eV and 0-20 meV), our calculations reveal the importance of many-body effects and their contributions to the desirable optical properties in the cubic organometallic perovskites system.

New insights into the diverse electronic phases of a novel vanadium dioxide polymorph: a terahertz spectroscopy study.

A remarkable feature of vanadium dioxide is that it can be synthesized in a number of polymorphs. The conductivity mechanism in the metastable layered polymorph VO2(B) thin films has been investigated by terahertz time-domain spectroscopy (THz-TDS). In VO2(B), a critical temperature of 240 K marks the appearance of a non-zero Drude term in the observed complex conductivity, indicating the evolution from a pure insulating state towards a metallic state. In contrast, the THz conductivity of the well-known VO2(M1) is well fitted only by a modification of the Drude model to include backscattering. We also identified two different THz conductivity regimes separated by temperature in these two polymorphs. The electronic phase diagram is constructed, revealing that the width and onset of the metal-insulator transition in the B phase develop differently from the M1 phase.