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- 实验方案
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Ultrafast Exciton Dissociation at the 2D-WS <sub/>2</sub> Monolayer/Perovskite Interface
摘要: In order for an excitonic photovoltaic (PV) device to perform efficiently, photogenerated excitons in the charge donor need to be dissociated through charge transfer (CT) to the acceptor rapidly after their photogeneration, and remain separated for a longer time to allow the collection of charges. To improve the efficiency of these steps, several combination of materials have been examined. Due to their excellent optical properties, two-dimensional transition metal dichalcogenides (2D-TMDs) have recently been explored. Another promising class of materials to platform efficient PVs is organic-inorganic perovskites. Here, we report on the ultrafast exciton dissociation through electron transfer from a 2D tungsten disulfide (WS2) monolayer to a thin layer of methylammonium lead iodide (CH3NH3PbI3) perovskites. Photoluminescence (PL) measurements showed that when the 2D-WS2 monolayer was covered with perovskites, its emission completely quenched, suggesting that the CT process is highly efficient. Despite that pump-probe spectroscopy measurements were carried out with a ~ 45 fs temporal resolution, the CT dynamics were not captured. A comparison of the ultrafast dynamics of the two band-edge excitons of the charge donor (2D-WS2) suggested that electron transfer is the dominant pathway of CT. Furthermore, these pump-probe measurements indicated that a small fraction of transferred electrons remained in the perovskites up to almost 2 ns. These findings may open a new horizon for understanding the dissociation of photogenerated excitons in 2D-TMD through hybridization with other class of nanomaterials.
关键词: Ultrafast Exciton Dissociation,Perovskite Interface,Hybrid Materials,Magnetic,Plasmonics,2D-WS2 Monolayer,Optical
更新于2025-09-23 15:21:01
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Time-resolved Element-selective Probing of Charge Carriers in Solar Materials
摘要: We review our recent results on the implementation of picosecond (ps) X-ray absorption spectroscopy to probe the electronic and geometric structure of centres formed by photoexcitation of solar materials such as polymorphs and inorganic Cs-based perovskites. The results show electron localization at Ti defects in TiO2 anatase and rutile and small hole polaron formation in the valence band of CsPbBr3, all within 80 ps. This method is promising for the study of the ultrafast time scales of such processes, especially with the advent of the Swiss X-ray Free Electron Laser (SwissFEL).
关键词: Solar materials,Ultrafast,Perovskites,X-ray absorption spectroscopy,TiO2
更新于2025-09-23 15:21:01
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Directly photoexcited Dirac and Weyl fermions in ZrSiS and NbAs
摘要: We report ultrafast optical measurements of the Dirac line-node semimetal ZrSiS and the Weyl semimetal NbAs, using mid-infrared pump photons from 86 meV to 500 meV to directly excite Dirac and Weyl fermions within the linearly dispersing bands. In NbAs, the photoexcited Weyl fermions initially form a non-thermal distribution, signi?ed by a brief spike in the differential re?ectivity whose sign is controlled by the relative energy of the pump and probe photons. In ZrSiS, electron-electron scattering rapidly thermalizes the electrons, and the spike is not observed. Subsequently, hot carriers in both materials cool within a few picoseconds. This cooling, as seen in the two materials’ differential re?ectivity, differs in sign, shape, and timescale. Nonetheless, we ?nd that it may be described in a simple model of thermal electrons, without free parameters. The electronic cooling in ZrSiS is particularly fast, which may make the material useful for optoelectronic applications.
关键词: ultrafast optical measurements,electronic cooling,photoexcitation,Dirac line-node semimetal,thermalization,Weyl semimetal
更新于2025-09-23 15:21:01
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Compressed Ultrafast Electron Diffraction Imaging Through Electronic Encoding
摘要: Ultrafast electron di?raction (UED) with high temporal and spatial resolutions is a powerful tool to observe transient structural changes in materials on an atomic scale. This technique is based on a pump-probe method using ultrashort laser and electron pulses. Therefore, UED requires that the measured transients be highly repeatable. Moreover, the relative time jitter between laser and electron pulses signi?cantly a?ects the UED temporal resolution. To overcome the UED technical limitations, we propose a technique called compressed ultrafast electron di?raction imaging (CUEDI). In this technique, we encode time-evolving electron di?raction patterns with random codes on an electron encoder. Then, the encoded electron di?raction pattern is measured by a detector after a temporal shearing operation. Finally, the evolution process of the electron di?raction pattern is reconstructed using a compressed sensing algorithm. We con?rm the feasibility of our proposed scheme by numerically simulating the polycrystalline gold melting process based on the experimental data measured with the pump-probe method. Because CUEDI employs a continuous or long electron pulse, the relative time jitter between laser and electron pulses can be eliminated. Additionally, CUEDI measures transients with a single shot, which allows irreversible processes to be directly observed.
关键词: compressed sensing,structural dynamics,single-shot measurement,Ultrafast electron di?raction
更新于2025-09-23 15:21:01
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Ultrafast dynamics observation during femtosecond laser-material interaction
摘要: Femtosecond laser technology has attracted significant attention from the viewpoints of fundamental and application; especially femtosecond laser processing materials present the unique mechanism of laser-material interaction. Under the extreme nonequilibrium conditions imposed by femtosecond laser irradiation, many fundamental questions concerning the physical origin of the material removal process remain unanswered. In this review, cutting-edge ultrafast dynamic observation techniques for investigating the fundamental questions, including time-resolved pump-probe shadowgraphy, ultrafast continuous optical imaging, and four-dimensional ultrafast scanning electron microscopy, are comprehensively surveyed. Each technique is described in depth, beginning with its basic principle, followed by a description of its representative applications in laser-material interaction and its strengths and limitations. The consideration of temporal and spatial resolutions and panoramic measurement at different scales are two major challenges. Hence, the prospects for technical advancement in this field are discussed finally.
关键词: ultrafast dynamics,ultrafast continuous optical imaging,femtosecond laser manufacturing,4D ultrafast scanning electron microscopy,pump-probe shadowgraphy
更新于2025-09-23 15:19:57
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Performance enhancement of graphene-coated micro heat pipes for light-emitting diode cooling
摘要: The rate of water transport through graphene nanocapillaries is profoundly enhanced compared to that in microscale capillaries due to the prevalence of exceptionally high capillary pressures and large slip lengths. As an inaugural study, we integrate graphene nanocapillaries into a micro heat pipe (MHP) for enhanced light-emitting diode (LED) cooling. With the use of graphene nanocapillaries, the ultrafast water transport synergically enhances the water circulation and evaporation process in the microfluidic device. The graphene-coated MHP achieves more than 45% enhancement in the overall performance compared to the uncoated counterpart. In turn, the experiments demonstrate a drastic reduction of LED’s operating temperature (more than 25 °C) which translates into a significantly prolonged lifespan of LED. The molecular dynamics simulations reveal that the oxygenated functional groups attached on graphene further increase the capillary pressure (~1000 bar) and effective velocity (~20 m/s) of the nanoconfined water, compared to those (~500 bar and ~10 m/s) in a pristine graphene nanochannel. The ultrafast water transport in graphene nanocapillary is justified. This study provides a holistic analysis and important insight into the phenomenon of ultrafast water transport in graphene nanocapillaries that exhibits an enormous potential in thermal energy management applications for LED cooling.
关键词: Electronics cooling,Micro heat pipe,Graphene nanocapillaries,Ultrafast water transport
更新于2025-09-23 15:19:57
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A Miniature Fibre-Optic Raman Probe Fabricated by Ultrafast Laser-Assisted Etching
摘要: Optical biopsy describes a range of medical procedures in which light is used to investigate disease in the body, often in hard-to-reach regions via optical fibres. Optical biopsies can reveal a multitude of diagnostic information to aid therapeutic diagnosis and treatment with higher specificity and shorter delay than traditional surgical techniques. One specific type of optical biopsy relies on Raman spectroscopy to differentiate tissue types at the molecular level and has been used successfully to stage cancer. However, complex micro-optical systems are usually needed at the distal end to optimise the signal-to-noise properties of the Raman signal collected. Manufacturing these devices, particularly in a way suitable for large scale adoption, remains a critical challenge. In this paper, we describe a novel fibre-fed micro-optic system designed for efficient signal delivery and collection during a Raman spectroscopy-based optical biopsy. Crucially, we fabricate the device using a direct-laser-writing technique known as ultrafast laser-assisted etching which is scalable and allows components to be aligned passively. The Raman probe has a sub-millimetre diameter and offers confocal signal collection with 71.3% ± 1.5% collection efficiency over a 0.8 numerical aperture. Proof of concept spectral measurements were performed on mouse intestinal tissue and compared with results obtained using a commercial Raman microscope.
关键词: Raman spectroscopy,ultrafast laser-assisted etching,micro-optics,optical biopsy
更新于2025-09-23 15:19:57
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Cuprous Sulfide for Different Laser Pulse Generation: Q-Switching and Mode-Locking
摘要: As a new type of copper-based chalcogenide two-dimensional nanomaterial, cuprous sulfide (Cu2S) has attracted much attention due to its unique band structure and optical properties. In this paper, all-fiber ring laser at the 1.53 μm regime with two kinds of Cu2S saturable absorber devices is demonstrated. The self-started Q-switched pulse with a central wavelength of 1530 nm was obtained for the first time by using Cu2S deposited on the fiber jumper as SA. When the tapered fibers deposited with Cu2S are used to replace the jumpers in the cavity, it can be found that the loss is significantly reduced and a mode-locked pulse with a pulse width of 896 fs has been achieved via evanescent field interaction. This experiment further enriches the application of Cu2S nanosheets in pulsed lasers and promotes the development and application of metal sulfides in nonlinear optics and ultrafast photonics.
关键词: saturable absorber,cuprous sulfide,mode-locking,Q-switching,ultrafast photonics,Cu2S,nonlinear optics
更新于2025-09-23 15:19:57
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41.8??W output power, 200??kHz repetition rate ultra-fast laser based on Yb:YAG single crystal fiber(SCF)amplifier
摘要: We demonstrate a high repetition rate, high energy chirped pulse amplification (CPA) system based on single crystal fiber (SCF) amplifier. With home-made all-fiber laser as the seed laser and Yb:YAG rod, SCF as the amplification gain medium, an output power of 61.8 W at 200 kHz repetition rate has been obtained. To the best of our knowledge, this is the highest power based on SCF at hundreds of kHz repetition rate. The measured M2 values are approximately 1.241 in the horizontal and 1.186 in the vertical direction. The spectrum width is 3.8 nm, which support Fourier transform-limited pulse duration of 411 fs. An average power of 41.8 W with pulse duration of 1.5 ps has been obtained after the chirped volume Bragg grating (CVBG) compressor, which will be compressed to hundreds of fs with accurate chirp compensation.
关键词: Ultrafast laser,SCF,Fiber laser,CPA
更新于2025-09-23 15:19:57
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Investigation of optical fiber-tip probes for common and ultrafast SERS
摘要: In this study, we performed a three-dimensional computational experiment on ultrashort pulse propagation in an optical fiber-tip probe that is decorated with gold nanoparticles (NPs) using a constant structure for the probe’s dielectric taper and different spatial configurations of the gold nanoparticles. Interestingly, a hot spot with the highest amplitude of the electric field was found not along the same chain of the NPs but between terminal NPs of neighboring chains of NPs at the probe’s tip (the amplitude of the electric field in the hot spots between the NPs along the same chain was of the order of 101, while that between terminal NPs of neighboring chains was of the order of 103). We eventually identified a configuration with only six terminal nanoparticles (Config4) which is characterized by the highest electric field amplitude enhancement and can provide the highest spatial resolution in the SERS interrogation of an object of interest. The ultrashort temporal responses of the hot spots for all configurations exhibited relatively high pulse elongation (relative elongation was greater than 4.3%). At the same time, due to the reflection of the incident pulse and consequent interference, the temporal responses of most hot spots contained several peaks for all configurations except for the optimum Config4. Nonetheless, the ultrashort temporal responses of all hot spots for Config4 were characterized by a single peak but with a relatively large pulse elongation (relative elongation was 234.1%). The results indicate that further examination of this new structure of a nanoparticles-coated optical fiber-tip probe with only six terminal NPs may provide attractive characteristics for its practical applications.
关键词: gold nanoparticles,femtosecond pulse,optical fiber-tip probe,ultrafast nanophotonics.,surface-enhanced Raman spectroscopy,temporal response
更新于2025-09-23 15:19:57