Anisotropic motion effects in CW non-linear EPR spectra: relaxation enhancement of lipid spin labels

Continuous-wave (CW) EPR measurements of enhancements in spin-lattice (T(1)-) relaxation rate find wide application for determining spin-label locations in biological systems. Often, especially in membranes, the spin-label rotational motion is anisotropic and subject to an orientational potential. We investigate here the effects of anisotropic diffusion and ordering on non-linear CW-EPR methods for determining T(1) of nitroxyl spin labels. Spectral simulations are performed for progressive saturation of the conventional in-phase, first-harmonic EPR signal, and for the first-harmonic absorption EPR signals detected 90 degrees -out-of-phase with respect to the Zeeman field modulation. Motional models used are either rapid rotational diffusion, or strong-jump diffusion of unrestricted frequency, within a cone of fixed maximum amplitude. Calculations of the T(1)-sensitive parameters are made for both classes of CW-experiment by using motional parameters (i.e., order parameters and correlation times), intrinsic homogeneous and inhomogeneous linewidth parameters, and spin-Hamiltonian hyperfine- and g-tensors, that are established from simulation of the linear CW-EPR spectra. Experimental examples are given for spin-labelled lipids in membranes.     

Technique for detecting changes in fluorescence lifetime by means of optoelectronic circuit auto-oscillation

We present a new, simple, inexpensive, and highly precise approach to excited-state fluorescence-lifetime-based measurements. The detection system consists of a closed-loop optoelectronic arrangement containing a radio frequency resonance amplifier, a fluorescence excitation light source, a fiber-optic delay line, and a photodetector. The system exhibits auto-oscillations in the form of intensity modulation. The oscillation frequency varies with the modulation phase shift of the fluorescent light. This frequency is used as the detection parameter, which is advantageous because frequency may be measured easily, inexpensively, and with high precision. This technique is well suited for chemical or biosensor applications.     

The continuous wave electron paramagnetic resonance experiment revisited

When the modulation frequency used in continuous wave electron paramagnetic resonance (cw EPR) spectroscopy exceeds the linewidth, modulation sidebands appear in the spectrum. It is shown theoretically and experimentally that these sidebands are actually multiple photon transitions, sigma(+)+kxpi, where one microwave (mw) sigma(+) photon is absorbed from the mw radiation field and an arbitrary number k of radio frequency (rf) pi photons are absorbed from or emitted to the modulation rf field. Furthermore, it is demonstrated that both the derivative shape of the lines in standard cw EPR spectra and the distortions due to overmodulation are caused by the unresolved sideband pattern of these lines. The single-photon transition does not even give a contribution to the first-harmonic cw EPR signal. Multiple photon transitions are described semiclassically in a toggling frame and their existence is proven using second quantization. With the toggling frame approach and perturbation theory an effective Hamiltonian for an arbitrary sideband transition is derived. Based on the effective Hamiltonians an expression for the steady-state density operator in the singly rotating frame is derived, completely describing all sidebands in all modulation frequency harmonics of the cw EPR signal. The relative intensities of the sidebands are found to depend in a very sensitive way on the actual rf amplitude and the saturation of single sidebands is shown to depend strongly on the effective field amplitude of the multiple photon transitions. By comparison with the analogous solutions for frequency-modulation EPR it is shown that the field-modulation and the frequency-modulation technique are not equivalent. The experimental data fully verify the theoretical predictions with respect to intensities and lineshapes.     

Sensitivity optimization in amplitude-modulated CW-EPR experiment

A sensitivity of recently developed method of amplitude-modulated continuous wave EPR (AM-CW-EPR) is studied depending on the parameters of the modulation field. The case of the significant saturation and high modulation frequency is addressed. It is found, that the rapid resonance passage effect is essential for AM-CW-EPR. However, its manifestation is different comparing to the conventional CW-EPR experiment. Both experimental data and numerical simulations support the enhancement of the AM-CW-EPR sensitivity under the rapid passage conditions for the modulating magnetic field, which is important for practical use of the method.     

Electromagnetically Induced Transparency and Absorption of A Monochromatic Light Controlled by a Radio Frequency Field

Electromagnetically induced transparency and absorption of a monochromatic light controlled by a radio frequency field in the cold multi-Zeeman-sublevel atoms are theoretically investigated. These Zeeman sublevels are coupled by a radio frequency(RF) field. Both electromagnetically induced transparency and electromagnetically induced absorption can be obtained by tuning the frequency of RF field for both the linear polarization and elliptical polarization monochromatic lights. When the transfer of coherence via spontaneous emission from the excited state to the ground state is considered, electromagnetically induced absorption can be changed into electromagnetically induced transparency with the change of intensity of radio field. The transparency windows controlled by the RF field can have potential applications in the magnetic-field measurement and quantum information processing.     

射频驱动下电磁诱导透明窗口的分裂和增益的出现

在Λ型三能级系统的基础上引入两个共振射频场, 通过详细讨论系统的探测吸收特性随两个射频场Rabi频率取不同值时的变化规律, 得出电磁诱导透明(EIT)的分裂规律以及EIT上出现增益现象的产生条件.研究结果表明: 两个射频场对系统所起的控制作用不同, 控制基态精细结构能级之间跃迁的射频场对EIT的分裂起作用, 而控制激发态精细结构能级之间跃迁的射频场不会导致EIT的分裂; 而且, 只有当控制基态精细结构能级之间跃迁的射频场的Rabi频率大于控制激发态精细结构能级之间跃迁的射频场的Rabi频率时, 才能产生EIT与增益相叠加的新特性. 关键词： 射频场 电磁诱导透明 增益 精细结构能级     

Harmonic detection with tunable diode lasers —two-tone modulation

The minimum absorption detectable by a tunable diode laser spectrometer utilising harmonic techniques is often limited by interference fringes generated by scattered light. The sensitivity of the spectrometer to absorption can be increased by applying a jitter modulation. In this paper, the theory of harmonic response for single- and two-tone modulation over optical fringes and Lorentzian absorption lines is developed and compared to experimental measurements. A simple analytic expression for the two-tone harmonic line shape is derived. This expression provides a physical understanding of the effects of the second modulation, and a means to unravel the effects of the second modulation on the linewidth and line shape. For a specific choice of the jitter frequency and phase, it is possible to simultaneously minimise the fringe signal and increase the harmonic absorption signal. The results of this investigation are applicable to trace gas detection using tunable diode lasers, and to other areas of spectroscopy and magnetic resonance where harmonic techniques are used.This work was supported by the Natural Sciences and Engineering Research Council of Canada, and the Ontario Ministry of the Environment     

Frequency stabilization of diode laser to 1.637μm based on the methane absorption line

The frequency of an external-cavity diode laser has been stabilized to 1.637 μm by using the reference of absorption lines of methane.The method can be applied to wavelength division multiplexed optical communication,fiber-optic sensing systems,as well as the high-sensitivity detection of methane.The derivative-like error signal yielded by frequency modulation and phase sensitivity detection technology is inputted into the PI feedback loop circuit in order to stabilize the frequency to the line center.After stabilization,the frequency fluctuation of diode laser is held within 5.6 MHz,and the root of Allan variance of error signal reaches a minimum of 1.66×10-10 for an average time of 10 s.     

利用非线性传输线产生高功率射频场

根据孤立子理论,分析了利用变容非线性传输线产生射频场的机理。利用电路仿真方法系统地研究了影响射频场产生的相关参数,发现电感和零压电容越小、输入电压越大,射频场的频率越高;电容的非线性率越大,射频场的峰值电压越高、高频成分越多。并在此基础上,仿真设计了能产生峰值功率为0.8 GW、主频为19.42 MHz射频场的非线性传输线。     

Comparison of CW-EPR and ESEEM technique for determination of water permeability profile in liposome membranes

The hydrophobicity profile across a membrane is an important parameter of biological membranes as it defines the barrier for permeation of polar molecules into the cell interior and of the stability of transmembrane proteins. In this work, the hydrophobicity profile was measured by conventional continuos-wave electron paramagnetic resonance (CW-EPR) and by electron spin echo envelope modulation (ESEEM) in two liposome suspensions with different ionic strengths in order to compare the sensitivity of both methods for the determination of the water penetration depth into the liposome membrane. Multilamellar liposomes from egg-phosphatidylcholine, cholesterol and dicetyl phosphate were prepared in deuterium oxide, buffered with phosphate buffer with or without NaCl at the phosphate concentrations 0.1 or 0.01 M. Liposomes were spin labeled with stearic acids spin probes with the nitroxide group at different positions on the acyl chain. The deuterium penetration depth was measured by the ESEEM technique and the signal was analyzed in the frequency domain (Fourier transform [FT]-ESEEM). The ratio of the intensities of FT-ESEEM lines at deuterium and hydrogen Larmor frequencies was used as a measures of the water penetration depth. It was also indirectly determined from the hyperfine splitting constants in frozen and in fluid state, measured by CW-EPR, as they depend on the polarity of the nitroxide group environment. The comparison of the two techniques demonstrated that FT-ESEEM is more sensitive to the changes on the surface of the membrane and thus more appropriate for the determination of the hydrophobic barrier than the conventional CW-EPR method.     

基于波长调制技术的激光器调制特性研究

在流场诊断技术中,可调谐半导体吸收光谱技术（TDLAS）成为主要的诊断技术之一,其可实现非接触、原位检测。波长调制（WMS）和直接吸收(DA)是两种最常用的TDLAS气体传感方法,在目标含量很低或者极端流场环境下,波长调制技术呈现出更多的优势,检测灵敏度与直接吸收相比可以提高1～2个数量级。在近红外波长调制技术应用领域,分布反馈式（DFB）半导体激光器成为流场诊断技术的光源选择之一,无论利用谐波信号（或者归一化谐波信号）的线型拟合,还是选择谐波信号的峰值来反演流场参数,吸收模型的准确建立均十分重要。在模型建立时,激光器频率-时间响应以及光强-时间响应的准确表示尤为重要。为解决吸收模型准确建立问题,提出了一种准确测量激光器调制参数的完整方法,通过实验测量了用于探测水汽吸收的1 392和1 469 nm激光器的调制特性,研究了分布反馈式激光器的调制参数随调制幅度,调制频率以及工作温度的变化。根据该方法得到的调制参数,建立吸收模型,测得常温下空气中水汽浓度为1.97%,直接吸收方法测得浓度为1.99%,验证了该测量方法的准确性。研究表明,调制深度随调制幅度的增加线性增加,随调制频率的增加非线性单调减小,随工作温度的升高线性增加;激光器的出光强度和频率同时被调制,强度变化超前频率变化的相位,随调制幅度的变化不明显,随调制频率的增加单调增加,随工作温度的升高单调减小;归一化一次谐波振幅和二次振幅均随调制幅度的增加而增加,随调制频率的增加而减小,随工作温度的变化不明显。在吸收光谱应用领域,波长调制技术发挥的作用愈加重要,调制系数与谐波信号的峰值息息相关,在波长调制技术应用时,选取适当的调制参数,有利于得到合适的谐波信号,可通过改变调制幅度、调制频率、工作温度得到最优调制系数。研究了近红外分布反馈式半导体激光器的调制特性,该方法同样适用于不同封装和不同波段激光器调制特性的研究,利于推广吸收光谱技术在各领域的应用。     

腔外多普勒频率调制激光稳频方法的研究

利用腔外气体吸收池内的SF_6分子饱和吸收线作为参考频率,并通过振动腔外反射镜使进入吸收池的激光的频率受到多普勒调制,实现了对CO_2激光10P(16)和10P(18)支线频率的闭环锁定,最大频率漂移约为7kHz.该法得到的稳频激光输出不仅无寄生频率调制和幅度调制,并且可将激光频率锁定在独立的分子吸收线中心.     

Correlation evolution and monogamy of two geometric quantum discords in multipartite systems

We study the controlled photon emission of generic V-type three-level molecules (e.g. BaF) via a radio frequency field. The density matrix approach was employed to calculate the probabilities of emission of one or two X-polarised photons. The influence of the relative delay phase between the sequential pulse on the emission photon probabilities can be enhanced or eliminated by the polarisation of the radio frequency field. For θ ∈ [ 0.35π,0.75π ] + nπ, the influence of the relative delay phase is enhanced, whereas for θ ? [ 0.35π,0.75π ] + nπ the influence is suppressed. The probabilities of emitting one or two X-polarised photons oscillate with the modulation index ζ, and several zero points exist, which could be used as a trigger for photon emissions. The results also demonstrated the phenomenon of radio frequency field-assisted photon absorption.     

磁绝缘线振荡器中空间电荷的调制

 首次研究了磁绝缘线振荡器中射频场（包括辐射波场和空间电荷波场）对空间电荷的调制,得到了在饱和时谐波电流一阶分量的公式。这个公式表明：考虑空间电荷波时,在小信号和辐射波与空间电荷波同相的条件下,它将增强谐波电流。在大信号时,情况不确定;谐波电流一阶分量将随二极管上电压的增加而增加,随运行频率和饱和长度的增加而减少。     

基于高精细度光腔锁频激光的分子吸收光谱测量

利用高精细度光腔锁定激光频率,实现了对分子吸收光谱的高精度测量.光腔采用低热膨胀系数的殷钢结构设计和温度控制,实现了腔长度的稳定;通过将激光频率锁定在光腔纵模上,实现了高频率精度和高灵敏度的光腔衰荡光谱测量.利用该装置示范性地测量了二氧化碳分子在6470.42 cm~(-1)附近的光腔衰荡光谱和色散光谱,得到了高精度的谱线参数,并和数据库谱线参数进行了对比.     

射频场控制的磁子能级中单色激光吸收抑制

理论上研究了射频场作用下多塞曼能级系统中单色激光的吸收抑制现象.一束单色线偏振或者椭圆偏振的激光作用于铷原子两能级间,线或椭圆偏振矢量方向与磁场方向垂直.在磁场中冷铷原子能级发生分裂,通过一个射频场将这些磁子能级耦合起来.当扫描射频场频率时,计算表明原子对单色光的吸收谱中出现了透射峰,类似于电磁诱导透明现象,光吸收减弱,光场透射增强.对于线性偏振或者椭圆偏振的单色光均能得到透射增强的结果 .这种现象完全不同于通常光泵磁共振实验中射频场与磁子能级谐振时光被吸收最多的现象.这种扫描射频场频率时单色光的透射增强现象来自于磁子能级间的相干效应.计算表明在扫描射频场频率时单色光吸收谱中出现的透射峰与射频场的拉比频率和椭圆偏振光的左旋和右旋圆偏振成分相关.这种射频场控制的单色光透射增强效应在磁场测量,光信息处理等领域有潜在的应用价值.     

射频场控制的磁子能级中单色激光吸收抑制

理论上研究了射频场作用下多塞曼能级系统中单色激光的吸收抑制现象.一束单色线偏振或者椭圆偏振的激光作用于铷原子两能级间,线或椭圆偏振矢量方向与磁场方向垂直.在磁场中冷铷原子能级发生分裂,通过一个射频场将这些磁子能级耦合起来.当扫描射频场频率时,计算表明原子对单色光的吸收谱中出现了透射峰,类似于电磁诱导透明现象,光吸收减弱,光场透射增强.对于线性偏振或者椭圆偏振的单色光均能得到透射增强的结果.这种现象完全不同于通常光泵磁共振实验中射频场与磁子能级谐振时光被吸收最多的现象.这种扫描射频场频率时单色光的透射增强现象来自于磁子能级间的相干效应.计算表明在扫描射频场频率时单色光吸收谱中出现的透射峰与射频场的拉比频率和椭圆偏振光的左旋和右旋圆偏振成分相关.这种射频场控制的单色光透射增强效应在磁场测量,光信息处理等领域有潜在的应用价值.     

电光晶体调谐的外腔反馈半导体激光器

报道一种用电光晶体实现快速调谐和凋制激光频率的方法.在Littrow型外腔反馈半导体激光中插入LiNbO3晶体,利用LiNbO3晶体的电光效应,通过改变晶体电压来调节激光器的有效腔长,可以对激光频率进行快速的调谐和调制.采用该方法,自制外腔反馈半导体激光器的调谐频率可达到2 kHz,它的调谐范围为350 MHz,激光频率调谐系数约为1.06 MHz/V,用饱和吸收光谱观测频率调谐的效果.快速激光频率调制可以应用在稳频技术上,将外腔反馈半导体激光器调制在5～100 kHz频率下,均获得了87Rb原子D2线的饱和吸收光谱的色散信号,并实现了激光频率在饱和吸收峰上的长期稳定.     

Intersubband absorption in modulation doped p-type Si1-xGex quantum wells: theory and experiment

A study of intersubband infrared absorption in modulation doped p-type Si/SiGe quantum wells is presented for SiGe wells with thicknesses between 22 Å and 64 Å and Ge contents in the range from 23% to 58%. The peak positions of the absorption lines are observed between 500 cm^-1 and 2200 cm^-1. Depending on the barrier height (i.e., on the Ge content of the wells), the heavy-hole states excited by the infrared radiation are either localized in the wells or strongly mixed with barrier-bound states and therefore delocalized. The shape of the absorption line correspondingly changes from a narrow Lorentz line to a rather broad absorption band. Using the structural parameters determined by high-resolution triple-axis x-ray diffraction, the results of a self-consistent Luttinger-Kohn type envelope function approach with the explicit inclusion of the strain in the quantum wells are in excellent agreement with the measured spectra.     

Frequency-dependent optical pumping in atomic ?-systems

We consider the effects of optical pumping on the conversion of laser-frequency modulation into intensity modulation by an atomic absorption line in a vapor of alkali atoms driven in a ?-configuration. It is found that, due to optical pumping in combination with the excited-state hyperfine structure, the absorption line shape is distorted substantially as the Fourier frequency of the FM is changed. The most significant effect of the distortion is a shift of the apparent line center, which depends on how the frequency of the modulation compares with the optical pumping rate. This shift has implications for locking lasers to atomic transitions and also for FM-AM noise conversion in atomic vapors.