- 标题
- 摘要
- 关键词
- 实验方案
- 产品
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Highly Conjugated, Fused-Ring, Quadrupolar Organic Chromophores with Large Two-Photon Absorption Cross-Sections in the Near-Infrared
摘要： The two-photon absorption (2PA) properties are investigated for two series of organic, π-conjugated, fused-ring, quadrupolar A-π-D-π-A chromophores of the type originally developed as non-fullerene acceptors for organic photovoltaics. These molecules are found to exhibit large nondegenerate two-photon absorption (ND2PA) cross-sections (ca. 6-27 × 103 GM) in the near infrared (NIR). In the first series, involving molecules of varying core size, ND2PA spectra and cross-sections characterized by femtosecond ND2PA spectroscopy in chloroform solutions reveal that increases in core size, and thus conjugation length, leads to substantially red-shifted and enhanced 2PA. In a second series, variation of the strength of the terminal acceptor (A) with constant core size (7 rings, indacene-based) led to less dramatic variation in the 2PA properties. Among the two core types studied, compounds in which the donor has a thieno[3,2-b]thiophene center demonstrate larger 2PA cross-sections than their indacene-centered counterparts, due to the greater electron-richness of their cores amplifying intramolecular charge transfer. Excited-state absorption (ESA) contributions to nonlinear absorption measured by open-aperture Z-scans are deduced for some of the compounds by analyzing the spectral overlap between 2PA bands and NIR ESA transitions obtained by ND2PA and transient absorption measurements, respectively. ESA cross-sections extracted from transient absorption and irradiance-dependent open-aperture Z-scans are in reasonable agreement and their moderate magnitudes (ca. 10-21 m2) suggest that, although ESA contributions are non-negligible, the effective response is predominantly instantaneous 2PA.
关键词： pump-probe spectroscopy,Nonlinear optics,Z-scan,organic optoelectronics,ultrafast spectroscopy,two-photon absorption
更新于2025-09-23 15:21:01
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Dual-comb-based asynchronous pump-probe measurement with an ultrawide temporal dynamic range for characterization of photo-excited InAs quantum dots
摘要： A dual-comb-based asynchronous optical sampling (ASOPS) pump-probe measurement system is demonstrated for characterizing the relaxation dynamics in a photo-excited self-assembled InAs quantum dot (QD) semiconductor. Although the photo-excited QD material has multiple complex relaxation processes, the transient transmittance responses (from femtoseconds to nanoseconds) are successfully obtained within a sub-second short acquisition time by using the ASOPS system. This is achieved with high stability and an extremely wide temporal dynamic range of approximately 105. The utility of the developed system is demonstrated as a powerful and easy-to-use measurement tool for studying the complex photo-excited dynamics of QD materials.
关键词： dual-comb,asynchronous optical sampling,InAs quantum dots,pump-probe measurement,relaxation dynamics
更新于2025-09-23 15:21:01
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A pump-probe scheme with a single chirped pulse to image electron and nuclear dynamics in molecules
摘要： A single chirped few-femtosecond pulse can be used to control and image coupled electron-nuclear dynamics. Using full ab initio simulations of the simplest molecule, H+2, as a prototype target, we show that for intermediate values of the chirp, interference between sequential and direct contributions enables significant control over ionization yields, even when taking into account the effective decoherence introduced by nuclear motion and the presence of an electronic continuum. For larger values of the chirp, the single chirped pulse reproduces a classical pump-probe setup, with the chirp parameter mapping an effective time delay between the pumping and probing frequencies of the pulse. After demonstrating this numerically, we present a full analytical solution for the two-photon ionization amplitudes that provides an intuitive analogy between the molecular dynamics induced by a single chirped pulse and a traditional pump-probe setup.
关键词： pump-probe scheme,attosecond science,chirped pulse,molecular ionization,electron-nuclear dynamics
更新于2025-09-23 15:21:01
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Many-particle excitations in non-covalently doped single-walled carbon nanotubes
摘要： Doping of single-walled carbon nanotubes leads to the formation of new energy levels which are able to participate in optical processes. Here, we investigate (6,5)-single walled carbon nanotubes doped in a solution of hydrochloric acid using optical absorption, photoluminescence, and pump-probe transient absorption techniques. We find that, beyond a certain level of doping, the optical spectra of such nanotubes exhibit the spectral features related to two doping-induced levels, which we assign to a localized exciton X and a trion T, appearing in addition to an ordinary exciton E1. We evaluate the formation and relaxation kinetics of respective states and demonstrate that the kinetics difference between E1 and X energy levels perfectly matches the kinetics of the state T. This original finding evidences the formation of trions through nonradiative relaxation via the X level, rather than via a direct optical excitation from the ground energy state of nanotubes.
关键词： exciton,doping,optical absorption,pump-probe transient absorption,photoluminescence,trion,single-walled carbon nanotubes
更新于2025-09-23 15:19:57
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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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[IEEE 2019 PhotonIcs & Electromagnetics Research Symposium - Spring (PIERS-Spring) - Rome, Italy (2019.6.17-2019.6.20)] 2019 PhotonIcs & Electromagnetics Research Symposium - Spring (PIERS-Spring) - Brillouin Optical Time Domain Analysis with Wavelength-locked Low-noise Pump-probe Laser Scheme
摘要： A doubly resonant short cavity Brillouin ring-laser actively stabilized with a wavelength locking system are employed as a low-RIN pump-probe source for Brillouin optical time-domain analysis (BOTDA) sensing. The developed high-stability narrow-linewidth laser scheme is compared to a long-cavity ring laser, showing the potential for enhanced temperature-strain resolutions.
关键词： wavelength-locked,temperature-strain resolutions,BOTDA,low-noise pump-probe laser,Brillouin Optical Time Domain Analysis
更新于2025-09-23 15:19:57
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Coherent Exciton Dynamics in Ensembles of Size-Dispersed CdSe Quantum Dot Dimers Probed via Ultrafast Spectroscopy: A Quantum Computational Study
摘要： Interdot coherent excitonic dynamics in nanometric colloidal CdSe quantum dots (QD) dimers lead to interdot charge migration and energy transfer. We show by electronic quantum dynamical simulations that the interdot coherent response to ultrashort fs laser pulses can be characterized by pump-probe transient absorption spectroscopy in spite of the inevitable inherent size dispersion of colloidal QDs. The latter, leading to a broadening of the excitonic bands, induce accidental resonances that actually increase the efficiency of the interdot coupling. The optical electronic response is computed by solving the time-dependent Schrodinger equation including the interaction with the oscillating electric field of the pulses for an ensemble of dimers that differ by their size. The excitonic Hamiltonian of each dimer is parameterized by the QD size and interdot distance, using an effective mass approximation. Local and charge transfer excitons are included in the dimer basis set. By tailoring the QD size, the excitonic bands can be tuned to overlap and thus favor interdot coupling. Computed pump-probe transient absorption maps averaged over the ensemble show that the coherence of excitons in QD dimers that lead to interdot charge migration can survive size disorder and could be observed in fs pump-probe, four-wave mixing, or covariance spectroscopy.
关键词： coherent electronic dynamics,pump-probe transient absorption spectroscopy,CdSe quantum dots dimers,exciton dynamics,size dispersion effects
更新于2025-09-23 15:19:57
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RECENT ADVANCES IN ULTRAFAST TIME-RESOLVED SCANNING TUNNELING MICROSCOPY
摘要： Making smaller and faster functional devices has led to an increasing demand for a microscopic technique that allows the investigation of carrier and phonon dynamics with both high spatial and temporal resolutions. Traditional optical pump–probe methods can achieve femtosecond temporal resolution but fall short in the spatial resolution due to the diffraction limit. Scanning tunneling microscopy (STM), on the contrary, has realized atomic-scale spatial resolution relying on the high sensitivity of the tunneling current to the tip-sample distance. However, limited by the electronics bandwidth, STM can only push the temporal resolution to the microseconds scale, restricting its applications to probe various ultrafast dynamic processes. The combination of these two methods takes advantages of optical pump–probe techniques and highly localized tunneling currents of STM, providing one viable solution to track atomic-scale ultrafast dynamics in single molecules and low-dimensional materials. In this review, we will focus on several ultrafast time-resolved STM methods by coupling the tunneling junctions with pulsed electric waves, THz, near-infrared and visible laser. Their applications to probe the carrier dynamics, spin dynamics, and molecular motion will be highlighted. In the end, we will present an outlook on the challenges and new opportunities in this field.
关键词： terahertz technique,femtosecond laser,Scanning tunneling microscopy,pump-probe technique,ultrafast dynamics.
更新于2025-09-19 17:15:36
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Ultrafast pump-probe ellipsometry and microscopy reveal the surface dynamics of femtosecond laser ablation of aluminium and stainless steel
摘要： An ultra-short laser pulse irradiated surface passes through a sequence of physical processes that occur over a wide temporal range, from femtoseconds to microseconds. In this paper for the first time, the complete laser ablation process for industrially relevant metals, aluminium (Al) and stainless steel (AISI 304) is tracked from the initial pulse impact to the final state. Time-resolved surface analytical techniques provide a complementary description of the surface dynamics. The pump-probe ellipsometry reveals changes of the complex refractive index for the first tens of picoseconds and time-resolved microscopy of the irradiated surface gives access to changes of the relative reflectivity from the initial femtosecond pulse impact to the final state at 10 μs. The changes in optical indices are affected by an ultrafast decrease in the density of the surface within the pressure unloading process in the first picoseconds and reveal spallation as the dominant mechanism for laser ablation in Al and stainless steel. The study also implies that the ablation volume is kept at an optimum when the ablation is initiated with ultrafast pulses within the pressure unloading process and is able to evolve over eight orders of magnitude without external perturbations.
关键词： Time-resolved ellipsometry,Spallation,Laser ablation,Nanostructure,Pump-probe reflectometry
更新于2025-09-19 17:13:59
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Implementation of data-cube pumpa??probe KPFM on organic solar cells
摘要： An implementation of pump–probe Kelvin probe force microscopy (pp-KPFM) is reported that enables recording the time-resolved surface potential in single-point mode or over a 2D grid. The spectroscopic data are acquired in open z-loop configuration, which simplifies the pp-KPFM operation. The validity of the implementation is probed by measurements using electrical pumping. The dynamical photoresponse of a bulk heterojunction solar cell based on PTB7 and PC71BM is subsequently investigated by recording point-spectroscopy curves as a function of the optical power at the cathode and by mapping 2D time-resolved images of the surface photovoltage of the bare organic active layer.
关键词： Kelvin probe force microscopy (KPFM),time-resolved measurements,bulk heterojunctions,organic photovoltaics,pump–probe configuration,photocarrier dynamics
更新于2025-09-16 10:30:52