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Carrier-Envelop Phase-Dependent Effect on Photoelectron Angular Distribution in Single-Cycle Laser Pulses * 下载免费PDF全文
Using a nonperturbative scattering theory, We study the photoelectron angular distributions (PADs) of Kr atoms irradiated by an infinite sequence of intense single-cycle pulses of circular polarization. We demonstrate the inversion asymmetry of PADs and the dependence of PADs on the carrier-envelop phase of the single-cycle pulses. The inversion asymmetry is caused by the interference between transition channels where the different channels are characterized by different combinations of absorbed-photon numbers in the ionization process. Our results provide a possible method to determine the value of carrier-envelop phase by the detected PADs. 相似文献
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High-Resolution Selective Excitation of Resonance-Enhanced Multiphoton-Ionization Photoelectron Spectroscopy by Shaping Femtosecond Laser Pulses 下载免费PDF全文
Femtosecond laser-induced resonance-enhanced multiphoton-ionization photoelectron spectroscopy (REMPI-PS) is faced with two drawbacks of low spectral resolution and poor selective excitation due to the broad spectral bandwidth. We propose a scheme to obtain a high-resolution selective excitation of (2+1) REMPI-PS by com- bining 7r and cosinusoidal phase modulation. Our theoretical results indicate that the (2+1) REMPI-PS signals related to neighboring excited states can be differentiated from their indistinguishable photoelectron spectra by the 7r phase modulation, and then their selective excitation can be realized by supplementally adding the cosi- nusoidal phase modulation. Furthermore, the physical mechanism of the high-resolution selective excitation of (2+1) REMPI-PS is explained by considering the two-photon power spectrum. 相似文献
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胆红素是人体胆汁中的主要色素,与人体健康密切相关.结合荧光蛋白的胆红素分子代表一类新型荧光发色团,在生物成像和生物传感领域有着重要应用.本文结合隐式溶剂模型和线性响应含时密度泛函理论方法计算了胆红素分子最低单重激发态的垂直激发能、振子强度和垂直发射能.以实验测量值和高水平RIADC(2)计算值作为参考,系统考察了一系列密度泛函方法的预测表现,结果发现最优化调控区间分离密度泛函方法整体表现最优,预测的绝对误差和相对误差最小.这得益于泛函中包含适宜的准确交换项比例能够产生既不离域也不局域的电子结构.在最优化调控泛函方法计算的波函数基础上,基于空穴-电子分析和片段间电荷转移方法定量表征了胆红素分子最低单重激发态,发现其具有杂化局域-电荷转移的激发特征.相信本工作可以为今后研究胆红素分子的激发态动力学过程和光谱性质提供重要理论依据,该最优化调控理论模型也可以为接下来其他生物分子体系的激发态性质研究提供可靠、高效的理论工具. 相似文献
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Simulating resonance-mediated two-photon absorption enhancement in rare-earth ions by a rectangle phase modulation 下载免费PDF全文
Improving the up-conversion luminescence efficiency of rare-earth ions via the multi-photon absorption process is crucial in several related application areas. In this work, we theoretically propose a feasible scheme to enhance the resonance-mediated two-photon absorption in Er~(3+) ions by shaping the femtosecond laser field with a rectangle phase modulation. Our theoretical results show that the resonance-mediated two-photon absorption can be decomposed into the on-resonant and near-resonant parts, and the on-resonant part mainly comes from the contribution of laser central frequency components, while the near-resonant part mainly results from the excitation of low and high laser frequency components.So, the rectangle phase modulation can induce a constructive interference between the two parts by properly designing the modulation depth and width, and finally realizes the resonance-mediated two-photon absorption enhancement. Moreover, our results also show that the enhancement efficiency of resonance-mediated two-photon absorption depends on the laser pulse width(or laser spectral bandwidth), final state transition frequency, and intermediate and final state absorption bandwidths. The enhancement efficiency modulation can be attributed to the relative weight manipulation of on-resonant and near-resonant two-photon absorption in the whole excitation process. This study presents a clear physical insight for the quantum control of resonance-mediated two-photon absorption in the rare-earth ions, and there will be an important significance for improving the up-conversion luminescence efficiency of rare-earthions. 相似文献
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Near-IR femtosecond lasers have been proposed to produce high-field terahertz radiation in the air via the laser-plasma interaction, but the physical mechanism still needs to be further explored. In this work, we theoretically investigate the effect of the two-color laser wavelength on the terahertz generation in the air based on a transient photocurrent model.We show that the long wavelength laser excitation can greatly enhance the terahertz amplitude for a given total laser intensity. Furthermore, we utilize a local current model to illustrate the enhancement mechanism. Our analysis shows that the terahertz amplitude is determined by the superposition of contributions from individual ionization events, and for the long wavelength laser excitation, the electron production concentrates in a few ionization events and acquires the larger drift velocities, which results in the stronger terahertz radiation generation. These results will be very helpful for understanding the terahertz generation process and optimizing the terahertz output. 相似文献
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发展精确、高效的交换-关联泛函一直是密度泛函理论工作者所追求的神圣目标。传统密度泛函被证实在计算原子或分子体系的某些基态和激发态性能时存在困难,而且预测不具有普适性;另一方面,一些高水平方法如耦合簇(CC)理论和基于格林函数(G)和屏蔽库仑作用(W)近似的多体微扰理论(MBPT),尽管相对精确但往往需要消耗昂贵的计算成本,因而其研究体系的尺寸和实用性受到了很大的限制。近年来,“最优化”调控区间分离泛函的发展在一定程度上使得上述问题得到改善,尤其是在消耗较少的计算成本前提下能够达到与高水平方法相媲美的预测精度,引起了越来越多的关注。本文首先简要回顾了密度泛函领域的理论背景,在区间分离密度泛函理论的基础上,重点介绍了最优化“调控”的概念;并且结合近期的理论工作对其在实际计算时的表现进行评价;最后,就最优化“调控”方法的前景和应用进行了展望。 相似文献