凝聚相中电子相干态的二维电子光谱测量（英文）

可见光波段的傅里叶变换二维电子光谱可用于对凝聚相分子复杂动力学过程的直接测量,包括量子相干现象.本文在对二维电子光谱原理的理解和对其物理本质更为直觉描述间做了一些铺垫,起到普及二维电子光谱的作用.重点阐述了二维电子光谱在测量电子相干态过程中是如何克服来自于量子力学原理的两大限制,即不确定性原理和测量导致的波包坍缩,并最终实现以本征态能级差为量子拍频的相干态测量.重点讨论了纯电子态相干、电子态与单模振动态耦合的相干,以及电子态与多模振动耦合形成的相干态所导致的复杂的量子相干现象.最后简要讨论了区分电子态相干及电子态-振动态耦合相干态的最新实验进展.     

基于主动锁相的二维电子光谱方法

二维电子光谱是探测复杂系统激发态相干动力学的重要工具,实现二维电子光谱测试的最大挑战是精确控制多束超短脉冲之间的相位差. 本综述回顾了利用主动相位管理方法实现二维电子光谱仪装置,主要包括干涉仪相位稳定、声光调制器进行频率标记和多光频梳等三类方法;结合四波混频、泵浦探测及完全共线等不同构型,能实现高时空分辨及量子跃迁通道选择的二维光谱检测. 超短脉冲技术与主动相位调控的结合实现二维电子光谱学方法,为研究激发态相干动力学提供新的机遇.     

基于主动锁相的二维电子光谱方法（英文）

二维电子光谱是探测复杂系统激发态相干动力学的重要工具,实现二维电子光谱测试的最大挑战是精确控制多束超短脉冲之间的相位差.本综述回顾了利用主动相位管理方法实现二维电子光谱仪装置,主要包括干涉仪相位稳定、声光调制器进行频率标记和多光频梳等三类方法;结合四波混频、泵浦探测及完全共线等不同构型,能实现高时空分辨及量子跃迁通道选择的二维光谱检测.超短脉冲技术与主动相位调控的结合实现二维电子光谱学方法,为研究激发态相干动力学提供新的机遇.     

基于金刚石体系中氮-空位色心的固态量子传感

在室温下,金刚石中的氮-空位(NV)色心具有荧光强度稳定、电子自旋相干时间长以及与生俱来的原子尺寸的特点,是优良的纳米量子传感器.在成像领域中,将各种超分辨成像显微技术应用于NV色心体系,发展出多种高空间纳米分辨率的成像方法.此外,NV色心作为固态量子比特可以通过光学方法对其进行初始化和读取.NV色心电子自旋量子态还可以与电磁场、应力等进行相干耦合.基于这些耦合,科研人员在实验上实现了对相关物理量纳米级空间分辨率的高灵敏表征.目前这些量子传感技术可以应用在新材料、单个蛋白质核自旋、活体神经元等方面的测量中.本综述主要介绍金刚石中NV色心纳米量子传感器件的工作原理、实验实现和优化以及在相关领域的应用.     

铷原子蒸气中超精细基态的双光子相干操控

二能级量子体系的相干操控对于精密测量和量子信息处理非常重要,如原子钟、原子干涉仪和量子计算等。在实验上观察到相干微波-射频(MW-RF)场驱动下的铷原子超精细基态的双光子Rabi振荡现象。基于塞曼子能级之间热弛豫过程的标定和微波跃迁的测量,清晰地分辨出叠加有热弛豫过程的原子态布居相干振荡。实验测得并详细讨论了广义Rabi频率与中间态失谐和微波/射频功率的关系。当中间态失谐较大时,实验结果与等效二能级理论模型非常吻合;但当中间态失谐较小时,少量原子占据中间态造成实测的Rabi频率偏离理论值。这些结果为二能级量子系统的相干操控提供了有力的理论支持。     

相干输运中的接点问题

为了研究介观体系的相干输运中接点的重要作用,采用一简单的纳米单势垒“二维-一维-二维”(2D-1D-2D)模型,应用散射矩阵方法和托马斯-费米近似,计算了体系透射率和在直流电压下电势分布. 结果表明： 1)接点对其透射率有显著的影响; 2)电势降落表现的电导性质违背了与经典串联电路中等价的基尔霍夫定律. 因此介观体系中各器件与接点间是量子相干的,考虑接点问题有利于对介观体系相干输运更为深入的研究. 关键词： 相干输运 接点 介观体系     

有序分子系统的线性与非线性光谱学的简化描述

通过对有序分子系统的线性与非线性光谱学的简化描述 ,帮助对有序分子体系光谱学进行研究的实验学家建立明确的物理图像和定量的研究工具 .这一描述是从最近对二阶非线性光学界面研究技术 ,即光学二次谐波 (SHG)和和频偏振振动光谱 (SFG VPS)的定量取向和偏振处理中推广出来的 .这一处理的方法关键在于简化线性和非线性光学中的有效极化率 ,构造出一个通用的取向泛函 ,并能通过实验参数清晰地计算出取向泛函的取向和强度因子 .同时还讨论了相干光谱技术在准确测量有序分子体系的取向和序的相比于非相干光谱方法的优点 .     

太赫兹辅助测量铷原子超快量子相干过程的理论研究

太赫兹辅助光电离瞬态测量方法可以分辨超快量子拍频,同时对复杂量子系统的超快密度矩阵演化进行成像.本文依据这种方法提出了一种具体的实验方案,利用紫外脉冲(脉宽为30 fs)和高强度太赫兹脉冲(峰值场强:约1 MV/cm)组成复合探测电场,探测铷原子5S1/2和5P3/2叠加态振荡周期约为2.6 fs的量子拍频过程,量子体系密度矩阵演化的布居项和相干项投影在光电子动量谱的不同位置,可以对密度矩阵演化实现完全信息测量.本文设计的实验方案不需要阿秒高次谐波或自由电子激光等复杂的先进光源,可以成为探索复杂量子体系超快相干动力学过程的新方案.     

二维系统研究中的无电极输运方法

介绍了两种极低温环境下无接触电极输运的测量方法—电容测量和表面声波测量.两种方法通过高频电场与电子的相互作用来研究量子系统体态的物理特性.首先介绍了在极低温下通过高精度电容测量研究高质量二维电子气特性的初步结果.实验装置具备在10 mK—300 K, 0—14 T环境中对小于1 pF的电容实现0.05%以上分辨率的能力.还介绍了利用表面声波研究二维电子系统的结果,可以在0.1 nW的输入激励下获得小于10^–5的灵敏度.这些测量手段在研究二维系统尤其是无法制作高质量接触电极的材料中具有广泛的应用前景.     

石墨烯中新奇量子物态的研究

石墨烯特殊的晶格结构和能带结构赋予了它独特的电学性质. 近年来, 分数量子霍尔态、 魔角石墨烯中的 关联绝缘体态和超导态等现象的发现不断证明着石墨烯是一种理想的二维模型体系, 可用于实现一系列新奇的量子物态, 对石墨烯中新奇量子物态的探测和调控也一直是凝聚态物理领域的前沿研究热点之一. 本文将系统地介绍近年来石墨烯中对称性破缺量子物态的研究进展, 包括平带中强关联量子物态的研究以及谷赝自旋调控的研究, 并介绍一种在纳米尺度、 单电子精度上探测二维材料体系简并度及对称性破缺态的普适方法, 希望为相关领域的研究人员提供参考和借鉴.     

捕光复合物中起源于电子-振动耦合的长时间相干

We theoretically investigate the evolutions of two-dimensional, third-order, nonlinear pho-ton echo rephasing spectra with population time by using an exact numerical path integral method. It is shown that for the same system, the coherence time and relaxation time of excitonic states are short, however, if the couplings of electronic and intra-pigment vibra-tional modes are considered, the coherence time and relaxation time of this vibronic states are greatly extended. It means that the couplings between electronic and vibrational modes play important roles in keeping long-lived coherence in light-harvesting complexes. Particularly, by using the method we can fix the transition path of the energy transfer in bio-molecular systems.     

Long-lived memory for mesoscopic quantum bits

We describe a technique to create long-lived quantum memory for quantum bits in mesoscopic systems. Specifically we show that electronic spin coherence can be reversibly mapped onto the collective state of the surrounding nuclei. The coherent transfer can be efficient and fast and it can be used, when combined with standard resonance techniques, to reversibly store coherent superpositions on the time scale of seconds. This method can also allow for "engineering" entangled states of nuclear ensembles and efficiently manipulating the stored states. We investigate the feasibility of this method through a detailed analysis of the coherence properties of the system.     

Theoretical study on the exciton dynamics of coherent excitation energy transfer in the phycoerythrin 545 light-harvesting complex

The experimental observation of long-lived quantum coherence in the excitation energy transfer(EET)process of the several photosynthetic light-harvesting complexes at low and room temperatures has aroused hot debate.It challenges the common perception in the field of complicated pigment molecular systems and evokes considerable theoretical efforts to seek reasonable explanations.In this work,we investigate the coherent exciton dynamics of the phycoerythrin 545(PE545)complex.We use the dissipation equation of motion to theoretically investigate the effect of the local pigment vibrations on the population transfer process.The result indicates that the realistic local pigment vibrations do assist the energy transmission.We demonstrate the coherence between different pigment molecules in the PE545 system is an essential ingredient in the EET process among various sites.The coherence makes the excitation energy delocalized,which leads to the redistribution of the excitation among all the chromophores in the steady state.Furthermore,we investigate the effects of the complex high-frequency spectral density function on the exciton dynamics and find that the high-frequency Brownian oscillator model contributes most to the exciton dynamic process.The discussions on the local pigment vibrations of the Brownian oscillator model suggest that the local heterogeneous protein environments and the effects of active vibration modes play a significant role in coherent energy transport.     

Phonon-assisted excitation energy transfer in photosynthetic systems

The phonon-assisted process of energy transfer aiming at exploring the newly emerging frontier between biology and physics is an issue of central interest.This article shows the important role of the intramolecular vibrational modes for excitation energy transfer in the photosynthetic systems.Based on a dimer system consisting of a donor and an acceptor modeled by two two-level systems,in which one of them is coupled to a high-energy vibrational mode,we derive an effective Hamiltonian describing the vibration-assisted coherent energy transfer process in the polaron frame.The effective Hamiltonian reveals in the case that the vibrational mode dynamically matches the energy detuning between the donor and the acceptor,the original detuned energy transfer becomes resonant energy transfer.In addition,the population dynamics and coherence dynamics of the dimer system with and without vibration-assistance are investigated numerically.It is found that,the energy transfer efficiency and the transfer time depend heavily on the interaction strength of the donor and the high-energy vibrational mode,as well as the vibrational frequency.The numerical results also indicate that the initial state and dissipation rate of the vibrational mode have little influence on the dynamics of the dimer system.Results obtained in this article are not only helpful to understand the natural photosynthesis,but also offer an optimal design principle for artificial photosynthesis.     

Quantum Transfer Energy and Nonlocal Correlation in a Dimer with Time-Dependent Coupling Effect

The presence of coherence phenomenon due to the interference of probability amplitude terms, is one of the most important features of quantum mechanics theory. Recent experiments show the presence of quantum processes whose coherence provided over suddenly large interval-time. In particular, photosynthetic mechanisms in light-harvesting complexes provide oscillatory behaviors in quantum mechanics due to quantum coherence. In this work, we investigate the coherent quantum transfer energy for a single-excitation and nonlocal correlation in a dimer system modelled by a two-level atom system with and without time-dependent coupling effect. We analyze and explore the required conditions that are feasible with real experimental realization for optimal transfer of quantum energy and generation of nonlocal quantum correlation. We show that the enhancement of the probability for a single-excitation transfer energy is greatly benefits from the combination of the energy detuning and time-dependent coupling effect. We investigate the presence of quantum correlations in the dimer using the entanglement of formation. We also find that the entanglement between the donor and acceptor is very sensitive to the physical parameters and it can be generated during the coherent energy transfer. On the other hand, we study the dynamical behavior of the quantum variance when performing a measurement on an observable of the density matrix operator. Finally, an interesting relationship between the transfer probability, entanglement and quantum variance is explored during the time evolution in terms of the physical parameters.     

ac Stark splitting and quantum interference with intersubband transitions in quantum wells

Resonant optical coupling experiments have demonstrated coherent quantum interference between the Stark-split "dressed states" of a synthesized 3-level electronic system in a semiconductor quantum well. Analysis of the dephasing mechanisms reveals dipole selection rules closely analogous to those seen in atomic spectroscopy experiments. In this respect, these systems behave as "artificial atoms" for the purposes of observing a range of nonclassical coherent optical effects. The prospects for exploiting them for scalable quantum information processing applications are more promising than previous dephasing models would have predicted.     

Expanding the view into complex material systems: From micro-ARPES to nanoscale HAXPES

The analysis of chemical and electronic states in complex and nanostructured material systems requires electron spectroscopy to be carried out with nanometer lateral resolution, i.e. nanospectroscopy. This goal can be achieved by combining a parallel imaging photoelectron emission microscope with a bandpass energy filter. In this contribution we describe selected experiments employing a dedicated spectromicroscope – the NanoESCA. This instrument has a particular emphasis on the spectroscopic aspects and enables laterally resolved photoelectron spectroscopy from the VUV up into the hard X-ray regime.     

Analysis of semiconductor surface phonons by Raman spectroscopy

Only recently Raman spectroscopy (RS) has advanced into the study of surface phonons from clean and adsorbate-covered semiconductor surfaces. RS allows the determination of eigenfrequencies as well as symmetry selection rules of surface phonons, by k-conservation limited to the Brillouin zone-center, and offers a significantly higher spectral resolution than standard surface science techniques such as high-resolution electron energy loss spectroscopy. Moreover, surface electronic states become accessible via electron–phonon coupling. In this article the fundamentals of Raman scattering from surface phonons are discussed and its potential illustrated by considering two examples, namely Sb-monolayer-terminated and clean InP(110) surfaces. Both are very well understood with respect to their atomic and electronic structure and thus may be regarded as model systems for heteroterminated and clean semiconductor surfaces. In both cases, localized surface phonons as well as surface resonances are detected by Raman spectroscopy. The experimental results are compared with surface modes predicted by theoretical calculations. On InP(110), due to the high spectral resolution of Raman spectroscopy, several surface modes predicted by theory can be experimentally verified. Surface electronic transitions are detected by changing the energy of the exciting laser light indicating resonances in the RS cross section. Received: 7 April 1999 / Accepted: 25 June 1999 / Published online: 16 September 1999     

不同维度ZnO能带结构和电子态密度的研究

本文采用基于密度泛函理论的第一性原理计算方法来研究不同维度ZnO的能带结构和电子态密度.参考实验上的ZnO晶格参数构建不同维度的ZnO模型并进行结构优化后再计算能带结构和电子态密度.研究结果表明二维和三维ZnO都属于直接带隙半导体且二维ZnO的禁带宽度大于三维ZnO;从三维变到二维,ZnO的电子局域化程度变高且Zn 3d轨道电子从能量较低的能级向能量较高的能级跃迁.本文的研究展示了二维和三维ZnO能带结构和电子态密度的异同,为二维ZnO基的器件研究提供了一定的理论参考价值.