On the relations of antibunching,sub-poissonian statistics and squeezing

The squeezing phenomenon is investigated in optical parametric processes and in Raman and hyper-Raman scattering. It is related to the antibunching effect and the sub-poissonian statistics of optical fields in these processes, and it is demonstrated that squeezing accompanies antibunching very often, but not always. In some cases squeezing may occur and antibunching may not and vice versa.     

Coherent anti-stokes raman scattering microscopy in the presence of electromagnetic confinement

The optical response used in studies of coherent anti-Stokes Raman scattering (CARS) microscopy can be enhanced or suppressed by means of electromagnetic confinement. In this paper, an approach based on planar mirrors is presented. Because of the classical origin of such a nonlinear optical effect, the theory is developed within a fully classical framework and it turns out that the CARS signal can be modified in a fashion similar to what has been extensively investigated for equivalent alterations of incoherent signals understood in terms of cavity quantum electrodynamics.     

光纤维中的喇曼混频

我们在656厘米^-1到1343厘米^-1的频率范围研究了光纤维的调谐喇曼混频(RM)效应。在实验中观察到下列现象:相干反斯托克斯喇曼散射(CARS)的大小与逆喇曼吸收(VRA)的大小成反比;RM对受激喇曼散射(SRS)的强度分布有强烈影响。除了观测到相干斯托克斯(CSRS)和CARS辐射,还观测到二级相干斯托克斯(SOCSRS)和相干反斯托克斯(SOCARS)辐射。对实验结果进行了讨论。 关键词：     

Time-resolved coherent anti-Stokes Raman scattering with a femtosecond soliton output of a photonic-crystal fiber

We demonstrate time-resolved coherent anti-Stokes Raman scattering (CARS) by using a frequency-tunable femtosecond soliton output of a silica photonic-crystal fiber (PCF) as a Stokes field. This approach allows quantum beats originating from two close Raman modes to be resolved in the time-domain CARS response. The nonresonant CARS background is efficiently suppressed by introducing a delay time between the probe pulse and the pump-Stokes pulse dyad, suggesting a convenient fiber-optic format for the Stokes source in time-resolved CARS and allowing sensitivity improvement in PCF-based CARS spectroscopes and microscopes.     

Achievement of Narrow-Band CARS Signal by Manipulating Broad-band Laser Spectrum

We theoretically demonstrate the achievement of narrow-band coherent anti-Stokes Raman scattering （CARS） signal by manipulating broad-band probe spectrum. The narrowing of the CARS signal depends on the spectrum bandwidth of the probe beam, and thus high-resolution CARS signal for a complicated quantum system can be obtained by the simple spectrum manipulation. Furthermore, the energy-level diagram for the complicated quantum system can also be labelled by measuring the CARS signal at a given frequency.     

Higher-Order Nonclassical Properties of a Shifted Symmetric Cat State and a One-Dimensional Continuous Superposition of Coherent States

Role of quantum interference in the origin of higher-order nonclassical characteristics of radiation field has been probed vis-à-vis a discrete and a continuous superposition of coherent states. Specifically, the possibilities of observing higher-order nonclassical properties (e.g., higher-order antibunching (HOA), higher-order sub-Poissonian photon statistics (HOSPS), higher-order squeezing (HOS) of Hong-Mandel type and Hillery type) have been investigated using a shifted symmetric cat state that reduces to Yurke-Stoler, even and odd coherent states at various limits. This shifted symmetric cat state which can be viewed as a discrete superposition of coherent states is found to show HOA and HOSPS. Similarly, higher-order nonclassical properties of a one-dimensional continuous superposition of coherent states is also studied here. The investigation has revealed the existence of HOS and HOSPS in the one-dimensional continuous superposition of coherent states studied here. Effect of non-Gaussianity inducing operations (e.g., photon addition and addition followed by subtraction) on these superposition states have also been investigated. Finally, some comparisons have been made between the higher-order nonclassical properties of discrete and continuous superposition of coherent states.     

Effects on squeezing and sub-poissonian of light in fourth harmonic generation up to first-order Hamiltonian interaction

The effects on squeezing and sub-poissonian of light in fourth harmonic generation (FHG) are investigated based on the fully quantum mechanically up to the first order Hamiltonian interaction in gt, where g is the coupling constant between the modes per second and t is the interaction time between the waves during the process in a nonlinear medium. FHG is a process in which an incident laser beam of the fundamental frequency ω interacts with a nonlinear medium to produce the harmonic frequency at 4ω. The coupled Heisenberg equations of motion involving real and imaginary parts of the quadrature operators are established. The occurrence of amplitude squeezing effects in both the quadratures of the radiation field in the fundamental mode is investigated and found to be dependent on the selective phase values of the field amplitude. The photon statistics of the pump mode in this process have also been investigated and found to be sub-poissonian in nature. It is found that there is no possibility to produce squeezed light in the harmonic mode up to first-order interaction in gt. Further, we have found the case up to second-order Hamiltonian interaction in gt that the normal squeezing in the harmonic mode is directly depends upon the fourth-order squeezing of the initial pump field. This gives a method of converting higher-order (fourth-order) squeezing into normal squeezing in the harmonic mode and vice versa.     

光场算符n次幂叠加激发混沌场的量子特性

构造了光场算符n次幂叠加激发混沌场,采用数值计算方法研究了该量子态的压缩效应、反聚束效应和统计性质,讨论了混沌场平均光子数、算符叠加系数及其幂次n对量子特性的影响.研究结果表明:光场算符n次幂叠加激发混沌场不呈现压缩效应,但呈现出反聚束效应和亚泊松分布性质,并且随平均光子数增大,它的反聚束效应和亚泊松分布性质减弱;随着算符组合部分中产生算符的比重增大,光场反聚束效应和亚泊松分布性质增强;随着算符幂次增大,亚泊松分布性质加强.     

Manipulating Nonclassicality via Quantum State Engineering Processes: Vacuum Filtration and Single Photon Addition

The effect of two quantum state engineering processes that can be used to burn a hole at vacuum in the photon number distribution of quantum states of radiation field is compared using various witnesses of lower- and higher-order nonclassicality as well as a measure of nonclassicality. Specifically, the modification in nonclassical properties due to vacuum state filtration and a single photon addition on an even coherent state, binomial state, and Kerr state are investigated using the criteria of lower- and higher-order antibunching, squeezing, and sub-Poissonian photon statistics. Further, the amount of nonclassicality present in these engineered quantum states having enormous applications in continuous variable quantum communication is quantified and analyzed by using an linear entropy-based entanglement potential. It is observed that all the quantum states studied here are highly nonclassical, and the hole-burning processes can introduce/enhance nonclassical features. However, it is not true in general. A hole at vacuum implies a maximally nonclassical state (as far as Lee's nonclassical depth is concerned), but a particular process of hole burning at vacuum does not ensure the existence of any particular nonclassical feature. Specifically, lower- and higher-order squeezing are not observed for photon-added and vacuum filtered even coherent states.     

Nonclassicality in off-resonant Raman process

The detuning parameter in experimentally feasible off-resonant Raman process is shown as a control parameter to probe and enhance the nonclassicality generated in the output of the process. Specifically, the normal characteristic function is obtained for the process as a function of detuning parameters in Stokes and anti-Stokes generation processes using more general solution than the conventional short-time solution under complete quantum treatment, which remains in the multimode Gaussian form. Single- and two-mode squeezing and antibunching as well as intermodal entanglement are reported in terms of experimentally accessible quantum noise fluctuations considering either phonon mode coherent or chaotic. Further, the joint photon-phonon number and integrated intensity distributions reveal a higher number of Stokes-phonon (pump-phonon) pair generation for the lower (higher) values of detuning parameter in Stokes generation. Pump-phonon pair generation is also supported by the lower values of detuning parameter in anti-Stokes generation.     

Molecularly sensitive optical coherence tomography

Molecular contrast in optical coherence tomography (OCT) is demonstrated by use of coherent anti-Stokes Raman scattering (CARS) for molecular sensitivity. Femtosecond laser pulses are focused into a sample by use of a low-numerical-aperture lens to generate CARS photons, and the backreflected CARS signal is interferometrically measured. With the chemical selectivity provided by CARS and the advanced imaging capabilities of OCT, this technique may be useful for molecular contrast imaging in biological tissues. CARS can be generated and interferometrically measured over at least 600 microm of the depth of field of a low-numerical-aperture objective.     

Ultrafast multiplex CARS investigation of vibrational characteristics in chloroform and PMMA

This paper demonstrates the femtosecond time-resolved coherent anti-Stokes Raman scattering by using folded BOXCARS geometry where an ultrashort broadband coherent white light continuum was used as Stokes pulse, and carries out the non-contact detection at long distance. The CARS signal is so easy to be detected that it can be seen even by nude eye. The C--H bonds of chloroform or PMMA were detected and the vibration modes belonging to the side chain and the main chain in PMMA were also compared. Their vibrational characteristics involved decay process and quantum beating were discussed. This modified CARS experimental technique could make up the deficiency of traditional CARS technique.     

Experimental Investigation on Selective Excitation of Two-Pulse Coherent Anti-Stokes Raman Scattering

Selective excitation of coherent anti-Stokes Raman scattering from the benzene solution is achieved by adaptive pulse shaping based on genetic algorithm, and second harmonic generation frequency-resolved optical gating （SHG-FROG） technique is adopted to characterize the original and optimal laser pulses. The mechanism for two-pulse coherent mode-selective excitation of Raman scattering is experimentally investigated by modulating the pump pulse in the frequency domain, and it is indicated that two-pulse coherent mode-selective excitation of Raman scattering mainly depends on the effective frequency components of the pump pulse related to specific vibrational mode. The experimental results suggest that two-pulse CARS has good signal-to-background ratio and high sensitivity, and it has attractive potential applications in the complicated molecular system.     

超衍射极限相干反斯托克斯拉曼散射显微成像技术及其探测极限分析

理论上提出一种突破衍射极限限制的相干反斯托克斯拉曼散射显微成像方法, 并对其探测极限进行分析.通过引入环形附加探测光与艾里斑周边的声子作用, 实现点扩展函数的改造, 提高相干反斯托克斯拉曼散射显微成像系统的横向空间分辨率. 随着分辨率的提高, 信号强度也随之降低, 尤其当应用于生物学、医学研究时, 样品分子数密度通常很低, 这将导致信号探测更加困难. 因此分析系统的探测极限, 确定超分辨体积元内的最小可探测分子数是展开超衍射极限相干反斯 托克斯拉曼散射显微成像实验研究的重要前提. 当泵浦光、斯托克斯光、探测光光强均达到极大值, 分辨率约40 nm三维空间内, 超衍射极限相干反斯托克斯拉曼散射显微成像系统的散粒噪声信噪比由曝 光时间与样品分子数密度决定. 曝光时间若取20 ms, 探测极限约为10³, 样品分子数目只有大于探测极限, 才能保证信号可以从噪声背景中提取出来. 关键词： 突破衍射极限 相干反斯托克斯拉曼散射 非线性光学 探测极限     

High-spectral-resolution coherent anti-Stokes Raman scattering with interferometrically detected broadband chirped pulses

To achieve high-spectral-resolution multiplex coherent anti-Stokes Raman scattering (CARS), one typically uses a narrowband pump pulse and a broadband Stokes pulse. This is to ensure a correspondence between anti-Stokes and vibrational frequencies. We obtain high-resolution CARS spectra of isopropanol, using a broadband chirped pump pulse and a broadband Stokes pulse, by detecting the anti-Stokes pulse with spectral interferometry. With the temporally resolved anti-Stokes signal, we can remove the chirp of the anti-Stokes pulse and restore high spectral resolution while also rejecting nonresonant scattering.     

Higher-order properties of photon-added coherent states

We have studied a higher-order squeezing and a higher-order sub-Poissonian photon statistics in photon-added coherent states. We obtained analytic forms of the degree of higher-order squeezing and the degree of higher-order sub-Poissonian statistics. We show that the photon-added coherent state |α,m〉 exhibits both higher-order squeezing and higher-order sub-Poissonian character. For two different types of higher-order squeezing, the degree of squeezing becomes bigger when the added photon number is increased. In single-photon-added coherent state, the degree of squeezing depends upon the order of squeezing N. When N is increased, the degree of squeezing becomes bigger in the Hong-Mandel-type higher-order squeezing but becomes smaller in the Hillery-type higher-order squeezing. Also, the higher-order sub-Poissonian character is more pronounced than the usual sub-Poissonian character in the single-photon-added coherent state.     

Molecular discrimination and contrast enhancement using a scanning coherent anti-stokes Raman microscope

New applications of a nonlinear optical microscope using coherent anti-Stokes Raman scattering (CARS) are presented. Excellent molecular discrimination using chemically similar molecular species and signal contrast enhancement using digital image processing are demonstrated. Limitations of the technique and future applications are discussed.     

Coherent anti-Stokes Raman spectroscopy (CARS)

By putting the non-linear susceptibility tensors in irreducible spherical form it is found that orientation averaging, selection rules, and the angular dependence of intensity on field polarizations all follow in a straightforward way. These spherical tensor techniques are used to treat coherent anti-Stokes Raman scattering (CARS) in detail and a comparison is made with conventional Raman scattering. The selection rules for both processes are shown to be the same. The paper concludes with a brief discussion of the rotational structure in CARS.     

The role of phase-matching and nanocrystal-size effects in three-wave mixing and CARS processes in porous gallium phosphide

Nonlinear-optical interactions, such as second-harmonic and sum-frequency generation and coherent anti-Stokes Raman spectroscopy (CARS), are investigated in porous GaP for the first time by means of a novel laser source based on mode-locked picosecond Nd³⁺:YVO₄ laser and subsequent continuum generation in an optical fiber. The efficiency of the former two nonlinear optical processes is shown to be strongly dependent on the wavelengths of the interacting waves and tends to increase with the decrease of the excitation wavelength. The power of the generated second-harmonic and sum-frequency increases by a factor of 2 and 30, respectively, compared to the crystalline GaP. In contrast, the CARS signal in porous GaP is found to be less efficient than one in crystalline GaP. The observed results are explained in terms of competition of the phase-matching effects in GaP nanocrystals and the enhanced photon lifetime in scattering porous GaP layers. PACS 42.25.Dd; 42.65.Ky; 42.70.Nq; 81.07.Bc