Delamination-Assisted Ultrafast Wrinkle Formation in a Freestanding Film.

Freestanding films provide a versatile platform for materials engineering thanks to additional structural motifs not found in films with a substrate. A ubiquitous example is wrinkles, yet little is known about how they can develop over as fast as a few picoseconds due to a lack of experimental probes to visualize their dynamics in real time on the nanoscopic scale. Here, we use time-resolved electron diffraction to directly observe light-activated wrinkling formation in freestanding La2/3Ca1/3MnO3 films. Via a "lock-in" analysis of oscillations in the diffraction peak position, intensity, and width, we quantitatively reconstructed how wrinkles develop on the time scale of lattice vibration. Contrary to the common assumption of fixed boundary conditions, we found that wrinkle development is associated with ultrafast delamination at the film boundaries. Our work provides a generic protocol to quantify wrinkling dynamics in freestanding films and highlights the importance of the film-substrate interaction in determining the properties of freestanding structures.

Strain-induced vibrational properties of few layer black phosphorus and MoTe2 via Raman spectroscopy.

We studied and compared the effect of tensile strain on the Raman spectra of black phosphorus (BP) and molybdenum ditelluride (MoTe2) crystals by using a simple custom strain device. In-situ Raman spectroscopy on BP revealed clear red shifting of all three phonon modes, A1 g, B2g and A2 g, under tensile stress. From our theoretical analyses, we found that such red shifting strongly depends on the direction of the strain exerted on the system even within the elastic deformation limit (i.e. strain ≤ 1 %). In particular, calculated results for the strain along the armchair direction are consistent with our experimental data, confirming that the strain applied to the sample acts effectively along the armchair direction. In a comparative study, we found that the effect of strain on the Raman shifting is larger for BP than that for MoTe2, presumably due to the smaller Young's modulus of BP. We also see a remarkable resemblance between donor-type intercalation induced vibrational properties and tensile stress-induced vibrational properties in BP. We anticipate that our method of in-situ Raman spectroscopy can be an effective tool that can allow observation of strain effect directly which is critical for future flexible electronic devices.

Layer-by-layer evolution of a two-dimensional electron gas near an oxide interface.

We report the momentum-resolved measurement of a two-dimensional electron gas at the LaTiO(3)/SrTiO(3) interface by angle-resolved photoemission spectroscopy (ARPES). Thanks to an advanced sample preparation technique, the orbital character of the conduction electrons and the electronic correlations can be accessed quantitatively as each unit cell layer is added. We find that all of these quantities change dramatically with distance from the interface. These findings open the way to analogous studies on other heterostructures, which are traditionally a forbidden field for ARPES.

Design and construction of a compact, high-repetition-rate ultrafast electron diffraction instrument.

We present the design and performance of a compact ultrafast electron diffraction instrument. The diffractometer provides a means of examining time-resolved ultrafast dynamical properties of solids. The system's utilization is discussed in terms of instrument parameters and diffraction data from selected condensed matter samples. The difractometer's performance is highlighted in terms of detection sensitivity, instrumental temporal resolution, and the electron beam transverse coherence length. Following specific details of the construction, we present a practical discussion of parameters such as repetition rate and provide advice on general construction approaches for laboratory-based, keV ultrafast electron diffractometers. In addition, design guidance for constructing a compact electron gun source that is well-suited for studying diffraction from hard condensed matter is given. A unique data acquisition scheme, utilizing high laser repetition rates, is presented.

Ultrafast manipulation of mirror domain walls in a charge density wave.

Domain walls (DWs) are singularities in an ordered medium that often host exotic phenomena such as charge ordering, insulator-metal transition, or superconductivity. The ability to locally write and erase DWs is highly desirable, as it allows one to design material functionality by patterning DWs in specific configurations. We demonstrate such capability at room temperature in a charge density wave (CDW), a macroscopic condensate of electrons and phonons, in ultrathin 1T-TaS2. A single femtosecond light pulse is shown to locally inject or remove mirror DWs in the CDW condensate, with probabilities tunable by pulse energy and temperature. Using time-resolved electron diffraction, we are able to simultaneously track anti-synchronized CDW amplitude oscillations from both the lattice and the condensate, where photoinjected DWs lead to a red-shifted frequency. Our demonstration of reversible DW manipulation may pave new ways for engineering correlated material systems with light.