Crystal Thickness Research Articles

The effect of melt drawing ratio on the crystal structural change and performance of polyketone extrusion cast film

In this paper, the polyketone (POK) extrusion cast film is manufactured by melt stretching method, and the evolution process of the crystal morphology and mechanical properties with the increase of melt drawing ratio (MDR) are followed. The results show that the melt stretching process produces many micro shish-kebab crystals in the POK. The length of the shish crystal and the thickness of the kebab crystal hardly increase with MDR, but the lateral length of the kebab crystal shows linear growth when MDR exceeds 40. The crystalline morphology of POK is mainly affected by melt relaxation. The molecular chain has sufficient relaxation during cooling at a low MDR (20–40). At this time, micro shish-kebab crystals are mainly randomly arranged. When MDR exceeds 40, the rapid melt stretching shortens the relaxation time of the tie chain between the neighborhood shish crystal, and the atomic force microscopy image shows a typical shish-kebab structure. This experimental result indicates that the formation of the oriented lamella structure may be related to the relaxation of the molecular chains between the micro-shish. When the length of the shish axis and the thickness of the kebab lamellae are similar, it is difficult to distinguish the two.

Controlling diffusion resistance, selectivity and deactivation of ZSM-5 catalysts by crystal thickness and defects

A systematic investigation of two sets of defect free and defective ZSM-5 crystals with controlled thickness (T) between 30 and 400 nm and of their performances in methanol conversion was reported for the first time in the present work. The defect free ZSM-5 crystals with a thickness of 35 nm are by far the smallest ever reported and displayed superior activity, stability and selectivity to slower diffusing compounds, which resulted in high yield of e.g. gasoline and the 1,2,4-trimethylbenzene isomer with high octane number, as compared to the other studied catalysts. Almost only products forming in the zeolite pores were detected and consequently, the external surface must be nearly inactive. Strong correlations between T and deactivation rate were observed. Thick crystals deactivated much faster than thin crystals, probably due to formation of carbon species in the zeolite pores, which results in pronounced percolation effects and faster deactivation of the former. At comparable thickness, crystals with defects deactivated much faster than defect free crystals, due to formation of additional small molecular coke species in the former. Strong correlations between T and selectivity were also observed and assigned to control of diffusion resistance by crystal thickness.

Pressure-Induced Superconductivity in HgTe Single-Crystal Film.

HgTe film is widely used for quantum Hall well studies and devices, as it has unique properties, like band gap inversion, carrier‐type switch, and topological evolution depending on the film thickness modulation near the so‐called critical thickness (63.5 Å), while its counterpart bulk materials do not hold these nontrivial properties at ambient pressure. Here, much richer transport properties emerging in bulk HgTe crystal through pressure‐tuning are reported. Not only the above‐mentioned abnormal properties can be realized in a 400 nm thick bulk HgTe single crystal, but superconductivity is also discovered in a series of high‐pressure phases. Combining crystal structure, electrical transport, and Hall coefficient measurements, a p‐n carrier type switching is observed in the first high‐pressure cinnabar phase. Superconductivity emerges after the semiconductor‐to‐metal transition at 3.9 GPa and persists up to 54 GPa, crossing four high‐pressure phases with an increased upper critical field. Density functional theory calculations confirm that a surface‐dominated topologic band structure contributes these exotic properties under high pressure. This discovery presents broad and efficient tuning effects by pressure on the lattice structure and electronic modulations compared to the thickness‐dependent critical properties in 2D and 3D topologic insulators and semimetals.

Ultra-broadband THz pulses with electric field amplitude exceeding 100 kV/cm at a 200 kHz repetition rate.

We demonstrate a table-top source delivering ultra-broadband THz pulses with electric field strength exceeding 100 kV/cm at a repetition rate of 200 kHz. The source is based on optical rectification of 23 fs pulses at 1030 nm delivered by a ytterbium-doped fiber laser followed by a nonlinear temporal compression stage. We generate THz pulses with a conversion efficiency of up to 0.11 % with a spectrum extending to 11 THz using a 1 mm thick GaP crystal and a conversion efficiency of 0.016 % with a spectrum extending to 30 THz using a 30 µm thick GaSe crystal. The essential features of the emitted THz pulse spectra are well captured by simulations of the optical rectification process relying on coupled nonlinear equations. Our ultrafast laser-based source uniquely satisfies an important requirement of nonlinear THz experiments, namely the emission of ultra-broadband THz pulses with high electric field amplitudes at high repetition rates, opening a route towards nonlinear time-resolved THz experiments with high signal-to-noise ratios.

Scaling effects in the alternating-current poling of thin PIN-PMN-PT single crystals

AC-poling of Pb(In1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 (PIN-PMN-PT) single crystals with a thickness of 0.06–0.16 mm was studied in this paper. Compared with DC-poled samples, enhancements in piezoelectric and dielectric properties can be obtained when the thickness is above 0.1 mm. However, inconsistency in poling effects was found in the crystals with thickness below 0.1 mm. To elucidate why such scaling effect arises, surface roughness was measured by an atomic force microscopy to correlate surface morphology and poling effects. It was found that non-uniform surface roughness led to inconsistent and decreased properties. Furthermore, temperature-dependent dielectric permittivity spectra were measured to explore how crystal thickness affects the thermal stability of ferroelectric phases. It is noted that complex changes in crystallographic symmetries emanate by decreasing thickness. Such phenomena can be attributed to more influential effects of surface morphology when thickness is reduced. We hope this work suggests a clue for solving the scaling effects of AC-poling on relaxor-PbTiO3 single crystals.

Bright and Dark States of Two Distant Macrospins Strongly Coupled by Phonons

We study the collective dynamics of two distant magnets coherently coupled by acoustic phonons that are transmitted through an intercalated crystal. By tuning the ferromagnetic resonances of the two magnets to an acoustic resonance of the crystal, we control a coherent three levels system. We show that the parity of the phonon mode governs the nature of the indirect coupling between the magnets: the resonances with odd / even phonon modes correspond to out-of-phase / in-phase lattice displacements at the magnets, leading to bright / dark states in response to uniform microwave magnetic fields, respectively. The sample is a tri-layer garnet consisting of two thin magnetic layers epitaxially grown on both sides of a half-millimeter thick non-magnetic single crystal. In spite of the relatively weak magneto-elastic interaction, the long lifetimes of the magnon and phonon modes in the sample are the key to unveil this long range strong coupling. This demonstrates that garnets are a great platform to study multi-partite hybridization process between magnon and phonons at microwave frequencies.

Terahertz Pulse Generation from GaAs Metasurfaces.

Ultrafast optical excitation of select materials gives rise to the generation of broadband terahertz (THz) pulses. This effect has enabled the field of THz time-domain spectroscopy and led to the discovery of many physical mechanisms behind THz generation. However, only a few materials possess the required properties to generate THz radiation efficiently. Optical metasurfaces can relax stringent material requirements by shifting the focus onto the engineering of local electromagnetic fields to boost THz generation. Here we demonstrate the generation of THz pulses in a 160 nm thick nanostructured GaAs metasurface. Despite the drastically reduced volume, the metasurface emits THz radiation with efficiency comparable to that of a thick GaAs crystal. We reveal that along with classical second-order volume nonlinearity, an additional mechanism contributes strongly to THz generation in the metasurface, which we attribute to surface nonlinearity. Our results lay the foundation for engineering of semiconductor metasurfaces for efficient and versatile THz radiation emitters.

Vertical Heterogeneous Integration of Metal Halide Perovskite Quantum-Wires/Nanowires for Flexible Narrowband Photodetectors

Charge collection narrowing (CCN) has been reported to be an efficient strategy to achieve optical filter-free narrowband photodetection (NPD) with metal halide perovskite (MHP) single crystals. However, the necessity of utilizing thick crystals in CCN limits their applications in large scale, flexible, self-driven, and high-performance optoelectronics. Here, for the first time, we fabricate vertically integrated MHP quantum wire/nanowire (QW/NW) array based photodetectors in nanoengineered porous alumina membranes (PAMs) showing self-driven broadband photodetection (BPD) and NPD capability simultaneously. Two cutoff detection edges of the NPDs are located at around 770 and 730 nm, with a full-width at half-maxima (fwhm) of around 40 nm. The optical bandgap difference between the NWs and the QWs, in conjunction with the high carrier recombination rate in QWs, contributes to the intriguing NPD performance. Thanks to the excellent mechanical flexibility of the PAMs, a flexible NPD is demonstrated with respectable performance. Our work here opens a new pathway to design and engineer a nanostructured MHP for novel color selective and full color sensing devices.

Two-dimensional recurrence relations and Takagi–Taupin equations. I. Dynamical X-ray diffraction by a perfect crystal

The dynamical diffraction of spatially restricted X-ray beams in a thick perfect crystal is studied using two-dimensional recurrence relations and the Takagi–Taupin (T-T) equations. It is shown that the two-dimensional recurrence relations are transformed into T-T equations when passing from a crystal with an array of discrete lattice planes to a model of continuous periodic electron density. The results of calculations of the X-ray diffraction field inside the crystal and the angular distribution of the scattering intensity in reciprocal space based on these two approaches are presented. It is shown that, when using the two-dimensional recurrence relations and T-T equations, the calculated contours of reciprocal-space maps and their qx sections are similar to each other, and the qz sections completely coincide.

Plate-like titanium silicalite-1 zeolites for green oxidation of alkenes to epoxides

Plate-like zeolites have attracted extensive attention due to their less molecular diffusion restriction. It is challenging to simultaneously control the high crystal aspect ratio and thin thickness. Here, two kinds of plate-like titanium silicalite-1 (TS-1) zeolites with crystal sizes of about 1.5 × 0.2 × 2.0 μm (a × b × c) and 0.3 × 0.06 × 0.6 μm were synthesized via assisted with crystal growth modifiers of citric acid and nitrilotriacetic acid, respectively. The 60 nm thickness was the thinnest TS-1 crystal among the reported by using crystal growth modifiers. The c/b aspect ratio of 10 was also one of the largest aspect ratios among the reported values for TS-1 crystals. Both of them displayed higher catalytic activities in 1-hexene epoxidation as compared with conventional nano-sized TS-1 catalysts.

Spectroscopy with Polarization Controlled Entangled Photons for Detecting Orbital Excitation in Solids

We propose an excitation-probe measurement method utilizing entangled photon pulses. The excitation-probe signal is dominated by stimulated Raman scattering as well as two-photon absorption when the time delay between the excitation pulse and the probe pulse is shorter than the pulseduration. This paper demonstrates that the two-photon-absorption signal can be suppressed when the photons of the pulses are entangled. The stimulated Raman scattering signal can be composed of many peaks distributed over broad photon energies owing to the transitions between numerous quantum states in complex materials. We also show that the desired peaks among the many peaks can be selected by controlling the thickness of the nonlinear crystal, the pump pulse center frequency,and the polarization of the excitation pulse and probe pulse.

Plate-Like ZSM-5 Zeolites as Robust Catalysts for the Cracking of Hydrocarbons.

Zeolites with good acid site accessibility and high diffusion rates are highly desirable catalysts, especially when dealing with bulk molecules. In this work, ZSM-5 zeolites with similar Si/Al ratios but different thicknesses along the b-axis (from ∼30 nm to ∼5 μm), namely, two plate-like ZSM-5 zeolites and two reference zeolites have been prepared and the impacts of b-axis thickness on the surface properties and catalytic cracking performances are explored. Comprehensive physiochemical studies demonstrate that reducing the b-axis thickness of the zeolite crystals endows the samples with better acid site accessibility and more external surface acid sites. Two model compounds with different molecule sizes, namely, 1,3,5-triisopropylbenzene (TIPB) and cumene, are selected to explore the catalytic cracking performances of the as-synthesized samples. The results reveal that decreasing the b-axis thickness of zeolite crystals can effectually promote the catalytic activity and stability in catalytic cracking reactions. For TIPB cracking, the greatly enhanced catalytic activity is ascribed to the enhanced acid site accessibility in plate-like ZSM-5 zeolites, and for cumene cracking, the improved catalytic stability is ascribed to the shortened diffusion length of plate-like zeolites.

Investigation on GaN-Based Membrane Photonic Crystal Surface Emitting Lasers.

A GaN-based blue photonic crystal surface emitting laser (PCSEL) featured with membrane configuration was proposed and theoretically investigated. The membrane dimension, photonic crystal (PhC) material, lattice constant and thickness were studied by RCWA (Rigorous Coupled Wave Analysis), FDTD (Finite Difference Time Domain) simulations with the confinement factor and gain threshold as indicators. The membrane PCSEL’s confinement factor of active media is of 13~14% which is attributed to multi-pairs of quantum wells and efficient confinement of the mode in the membrane cavity with air claddings. The excellent confinement factor and larger Q factor of resonance mutually contribute to the lower gain threshold of the design (below 400 cm−1 for GaN-PhC with 100 nm thick top and bottom GaN layer, 40 nm hole radius and 40 nm depth). The PhC confinement factor exceeds 13% and 6% for TiO2-PhC with 80 nm and 60 nm PhC thickness and 20 nm and 40 nm distance between PhC and active media, respectively. It is around two times larger than that of GaN-PhC, which is attributed to the higher refractive index of TiO2 that pulls field distribution to the PhC layer.

Optimization of highly oriented pyrolytic graphite applied to neutron crystal optics

The neutron diffraction properties of highly oriented pyrolytic graphite (HOPG) are reviewed using experimental results that have been obtained by diffraction of high-energy gamma rays, X-rays and neutrons. The interpretation of the empirical data based on diffraction theory leads to generic diagrams that display the performance of HOPG as a function of crystal thickness, mosaic spread and neutron wavelength. The analysis of the relation between the defect structure and diffraction properties demonstrates the usefulness of a detailed X-ray diffraction study to maximize the efficiency of composite neutron monochromators and analyzers. The optimization procedure is illustrated by the configuration of a double-focusing monochromator.

High-rate OVPE-GaN crystal growth at a very high temperature of 1300 °C

Polycrystal formation is an issue to be resolved to grow thick GaN crystals by the oxide vapor phase epitaxy (OVPE) method. Since the high-temperature growth at 1250 °C was effective in suppressing the polycrystal formation in our previous study, we attempt further high-temperature OVPE-GaN crystal growth at 1300 °C. However, the GaN surface decomposition becomes severe at 1300 °C. The pre-growth epitaxy was employed to avoid surface decomposition and enable high-temperature growth. Nearly polycrystal-free growth of GaN crystal was achieved, and we obtained a 478 μm thick OVPE-GaN layer at 1300 °C with a further high growth rate of about 200 μm h−1.

A study on the growth process for liquid phase epitaxy of GaN crystal using Na–Li–Ca flux

The liquid epitaxial growth process on the HVPE-GaN seed of GaN crystal was investigated using the Na–Li–Ca flux method. The phase structure and morphology of as-grown GaN crystals were characterized by X-ray diffraction (XRD) and the scanning electron microscope (SEM), respectively. Under the growth time of 70h, a large area of dissolution morphology could be observed accompanied by a decrease in the thickness of the HVPE-GaN seed. At the bottom of the crucible, the thinning of the seed crystal thickness was the most obvious. For the growth time of 150h, there were two kinds of appearances along the height direction, presenting gathered ridges in the upper part and cellular organizations in the middle and bottom parts. For 420h, the as-grown crystal presented a typical hexagonal layered morphology and the side face developed outward forming regular hexagonal crystallographic planes. With prolonging time from 150h to 420h, the LPE growth shifted from non-equilibrium growth mode with an unstable cellular growth surface morphology to near-equilibrium growth mode with a typical hexagonal layered growth morphology. The thickness of as-grown crystal showed a decrease trend from the gas-liquid interface to the bottom of crucible. To get near-equilibrium growth mode for the whole crystal plate in Na-flux method, the promotion of N dissolving, GaN growth unit diffusion is the key issue.

Effect of front, lateral and back dead layer thicknesses of a HPGe detector on full energy peak efficiency

As well known, High Purity Germanium (HPGe) detectors have a wide range of applications in every area where radiation detection and measurements are involved. One of the most important parameters in this respect is the determination of the full energy peak (FEP) efficiency. There are certain parameters affecting the so-called FEP efficiency. Perhaps the most important one is the thickness of dead layers of the crystal itself. In the current study, we investigated the effects of the thickness of front, lateral and back dead layer thicknesses of the detector crystal on the FEP efficiencies for the energy range 30 keV–5 MeV using EGS4 Monte Carlo simulation package. It was shown that the change in the thickness of the front dead layer has significant effect on the efficiency values for the energy interval 30–400 keV. The change in the thickness of the lateral and back dead layer was shown to have significant effects on the efficiencies for the energy intervals 2–3 MeV and 3–5 MeV, respectively. The results were checked using GEANT4 and a good agreement was observed.

Evolutionary 2D organic crystals for optoelectronic transistors and neuromorphic computing

Abstract Brain-inspired neuromorphic computing has been extensively researched, taking advantage of increased computer power, the acquisition of massive data, and algorithm optimization. Neuromorphic computing requires mimicking synaptic plasticity and enables near-in-sensor computing. In synaptic transistors, how to elaborate and examine the link between microstructure and characteristics is a major difficulty. Due to the absence of interlayer shielding effects, defect-free interfaces, and wide spectrum responses, reducing the thickness of organic crystals to the 2D limit has a lot of application possibilities in this computing paradigm. This paper presents an update on the progress of 2D organic crystal-based transistors for data storage and neuromorphic computing. The promises and synthesis methodologies of 2D organic crystals (2D OCs) are summarized. Following that, applications of 2D OCs for ferroelectric non-volatile memory, circuit-type optoelectronic synapses, and neuromorphic computing are addressed. Finally, new insights and challenges for the field’s future prospects are presented, pushing the boundaries of neuromorphic computing even farther.

Topological magnetic hysteresis in single crystals of CeAgSb2 ferromagnet

Closed-topology magnetic domains are usually observed in thin films and in an applied magnetic field. Here we report the observation of rectangular cross-section tubular ferromagnetic domains in thick single crystals of CeAgSb2 in zero applied field. Relatively low exchange energy, small net magnetic moment, and anisotropic in-plane crystal electric fields lower the domain wall energy and allow for the formation of the closed-topology patterns. The tubular domain structure irreversibly transforms into a dendritic pattern upon cycling the magnetic field. This transition between closed and open topologies results in a ‘topological magnetic hysteresis’— the actual hysteresis in magnetization, not due to the imperfections and pinning, but due to the difference in the pattern morphology. Similar physics was suggested before in pure type-I superconductors and is believed to be a generic feature of other nonlinear single (present case), or two-phase (type-I superconductor) systems where the effects similar to demagnetization (shape-dependent macroscopic variation of properties) lead to pattern formation.

Geometric progress in the thickness of exfoliated van der Waals crystals on the example of MoS2

To obtain molecularly thin flakes via mechanical exfoliation from a bulk layered crystal, the process should be repeated multiple times, but the mathematical principle behind this phenomenon remains unknown. In this paper, we show how the thickness of the MoS2 flake changes with subsequent cleavages of the adhesive tape, with the tests carried out on two widely used dicing tapes and Scotch removable tape. In the beginning, we assumed that with each subsequent tear of the tape, the thickness of the material decreases by half. We discovered that the exfoliated crystal thickness decreases with geometric progress and proposed a formula depicting that phenomenon. In addition, the exfoliated flakes are observed to crumble during the process and the fragmentation factor is discussed as well. Our observations will allow for more efficient estimation of the number of steps required to produce a sample of the desired thickness, relevant for tuning electronic transport properties and optical activity of two-dimensional materials.