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Theoretical and experimental investigation of UV–Vis absorption spectra in plasma-activated water 等离子体活化水中UV-Vis吸收光谱的理论与实验研究
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-10-14 DOI: 10.1140/epjd/s10053-025-01074-y
Nilton F. AzevedoNeto, Orisson P. Gomes, Felipe S. Miranda, Paulo N. Lisboa-Filho, Augusto Batagin-Neto, Didier Bégué, Rodrigo S. Pessoa

This research comprehensively examines the physicochemical and optical properties of plasma-activated water (PAW) produced by a serially associated dielectric barrier discharge (DBD) and gliding arc plasma jet (GAPJ) system. Experimental UV–Vis spectroscopy identified prominent absorption bands attributed to reactive oxygen and nitrogen species (RONS) such as nitrite (NO2), nitrate (NO3), hydrogen peroxide (H2O2), nitrous acid (HNO2), and nitric acid (HNO3). To precisely interpret the complex and overlapping experimental spectra, density functional theory (DFT) simulations were utilized to model electronic transitions. These theoretical findings crucially revealed the influence of protonation on the optical features, showing blue-shifted bands for ionic species and red-shifted bands for their protonated forms.

Graphic abstract

Integrated UV-Vis and TD-DFT analysis of Plasma-Activated Water (PAW) from a serial DBD-GAPJ system, highlighting the decisive influence of protonation on the optical features of RONS

本研究全面考察了介电阻挡放电(DBD)和滑动电弧等离子体射流(GAPJ)串联相关系统产生的等离子体活化水(PAW)的物理化学和光学特性。实验紫外-可见光谱发现,亚硝酸盐(NO2−)、硝酸盐(NO3−)、过氧化氢(H2O2)、亚硝酸(HNO2)和硝酸(HNO3)等活性氧和氮物质(RONS)的显著吸收带。为了精确解释复杂和重叠的实验光谱,利用密度泛函理论(DFT)模拟电子跃迁。这些理论发现至关重要地揭示了质子化对光学特性的影响,显示了离子种类的蓝移带和质子化形式的红移带。图摘要对连续DBD-GAPJ系统的等离子体活化水(PAW)进行了UV-Vis和TD-DFT综合分析,突出了质子化对RONS光学特性的决定性影响
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引用次数: 0
The energy dependence of the rotational relaxation process in the collision between excited state H2 X1Σg+(v = 1, J = 9, 11) and CO 激发态H2 X1Σg+(v = 1, J = 9,11)与CO碰撞时旋转弛豫过程的能量依赖
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-10-08 DOI: 10.1140/epjd/s10053-025-01075-x
Kai Wang, Zhong Liu, Shuying Wang, Xinru Li

The collisional relaxation between excited H2 and CO is investigated utilizing the stimulated Raman pumping (SRP) technique to achieve the excited state of H2 X1Σg+(v = 1, J = 9, 11). The excitation to the H2(1, 9) (E = 5900 cm−1) and H2(1, 11) (E = 6245 cm−1) energy levels were confirmed using coherent anti-Stokes Raman spectroscopy (CARS). At a sample cell temperature of 298 ± 1 K, the collisional depopulation rate of H2(1, J) molecules was obtained by fitting the graph of CARS signal intensity versus delay time. The collisional transfer rate coefficients between excited H2(1, J) molecules and CO, under varying excitation energy conditions, were calculated using the Stern–Volmer equation. For J = 9, the rate coefficients were kJ=9(CO) = (2.36 ± 0.55) × 10–14 cm3 s−1 and kJ=9(H2) = (0.89 ± 0.29) × 10–14 cm3 s−1, while for J = 11, they were kJ=11(CO) = (1.90 ± 0.36) × 10–14 cm3 s−1 and kJ=11(H2) = (0.65 ± 0.19) × 10–14 cm3 s−1. It was observed that the collisional transfer rate coefficient decreased with increasing excitation energy. When the cell temperature was varied from 298 to 475 K, the collisional transfer rate coefficients for the H2-CO system increased nonlinearly with temperature. Analysis of the time-resolved CARS spectra for individual rotational levels of H2(1, J) demonstrated that multi-quantum transitions with ΔJ = 4 dominated during relaxation. Furthermore, the higher excitation energy is linked to the longer relaxation times to achieve equilibrium. Elevating the temperature of the cell significantly accelerated the relaxation process, and the rotation-rotation (R-R) energy transfer process exhibited high-temperature sensitivity. The time evolution of the rotational temperature for H2(1, 9) molecules was determined using the Boltzmann rotational distribution. The rotational temperature decayed exponentially, eventually stabilizing within the 362–379 K range.

Graphical Abstract

利用受激拉曼泵浦(SRP)技术研究了H2与CO之间的碰撞弛豫,以获得H2 X1Σg+(v = 1, J = 9,11)的激发态。利用相干反斯托克斯拉曼光谱(CARS)证实了H2(1,9) (E = 5900 cm−1)和H2(1,11) (E = 6245 cm−1)能级的激发。在样品细胞温度为298±1 K时,通过拟合CARS信号强度随延迟时间的变化曲线,得到H2(1,j)分子的碰撞失居率。利用Stern-Volmer方程计算了不同激发能条件下H2(1, J)分子与CO的碰撞传递速率系数。J = 9,系数kJ = 9 (CO) =(2.36±0.55)×10 - 14立方厘米−1和kJ = 9 (H2) =(0.89±0.29)×10 - 14立方厘米−1,而对于J = 11,他们kJ = 11 (CO) =(1.90±0.36)×10 - 14立方厘米−1和kJ = 11 (H2) =(0.65±0.19)×10 - 14立方厘米−1。结果表明,碰撞传递率系数随激发能的增大而减小。当电池温度在298 ~ 475 K范围内变化时,H2-CO体系的碰撞传递速率系数随温度呈非线性增加。对H2(1, J)各个旋转能级的时间分辨CARS光谱分析表明,在弛豫过程中,ΔJ = 4的多量子跃迁占主导地位。此外,较高的激发能与较长的松弛时间相关联,以达到平衡。升高细胞温度可显著加速弛豫过程,旋转-旋转(R-R)能量传递过程表现出高温敏感性。利用玻尔兹曼旋转分布确定了H2(1,9)分子的旋转温度随时间的变化。旋转温度呈指数衰减,最终稳定在362 ~ 379 K范围内。图形抽象
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引用次数: 0
Cellular DNA damage induced by low-energy (0–20 eV) electrons 低能电子(0-20 eV)诱导的细胞DNA损伤
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-10-07 DOI: 10.1140/epjd/s10053-025-01069-9
Léon Sanche

In this article, different types of experiments are suggested to further investigate the interactions of low-energy (0–20 eV) electrons (LEEs) with DNA under conditions increasingly closer to those of living cells. Their feasibility is illustrated by describing the methods involved, together with recently obtained results. These include LEE-impact experiments on plasmid films surrounded by water and oxygen or modified to account for the presence of amino acids bound to DNA in the nucleus. Measurements of cellular behavior due to DNA damage induced by LEEs generated outside or inside the cell are also described. The former shows a direct correspondence between the decay of core-excited transient anions into destructive channels and the decrease of cellular functionality. Using femtosecond lasers, it is also possible to directly probe the action of LEEs in living cells. In these experiments, the LEE energy distribution in the cellular medium and the time required for the biological response must be considered. The generation of LEE distributions is discussed in terms of the present limit of stochastic model calculations to include the quantum behavior of LEEs, and the biological response, which requires considerable knowledge of the molecular biology involved to reach a detailed interpretation of the dose–response curves. An improved fundamental understanding of the action of LEEs in the cell nucleus is expected to assist in the targeting of radiosensitizing molecules toward the most vulnerable sites in DNA and hence improve chemoradiation therapy.

Graphical Abstract

Analysis of cell behavior following low energy electron (LEE) impact from a direct source and that generated from a femtosecond laser

本文建议在越来越接近活细胞的条件下,进行不同类型的实验来进一步研究低能电子(0-20 eV)与DNA的相互作用。通过描述所涉及的方法以及最近获得的结果,说明了它们的可行性。这些实验包括对被水和氧包围的质粒膜进行LEE-impact实验,或者对其进行修饰以解释细胞核中与DNA结合的氨基酸的存在。还描述了由细胞内外产生的LEEs引起的DNA损伤引起的细胞行为的测量。前者显示了核激发的瞬态阴离子向破坏通道的衰变与细胞功能的下降之间的直接对应关系。利用飞秒激光,还可以直接探测活细胞中LEEs的作用。在这些实验中,必须考虑细胞介质中的LEE能量分布和生物反应所需的时间。根据目前随机模型计算的极限来讨论LEE分布的产生,以包括LEE的量子行为和生物反应,这需要相当多的分子生物学知识来达到剂量-反应曲线的详细解释。提高对LEEs在细胞核中的作用的基本理解有望有助于将放射致敏分子靶向DNA中最脆弱的部位,从而改善放化疗。图解【摘要】分析了直接源和飞秒激光产生的低能电子(LEE)冲击后的电池行为
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引用次数: 0
Momentum flux measurements in a negative ion beam for fusion research 用于核聚变研究的负离子束流动量通量测量
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-10-07 DOI: 10.1140/epjd/s10053-025-01053-3
Thomas Trottenberg, Alexander Spethmann, Loïc Schiesko, Christian Wimmer, Holger Kersten, Ursel Fantz

A new method for determining the particle flux density in the beam of a neutral beam injector (NBI) for magnetically confined fusion plasmas is presented. The method uses a force probe to measure the momentum transfer from beam particles to a small target and has been applied at the BATMAN experimental facility at the MPI Garching. The experiments presented in this report are performed in the non-neutralized negative ion beam. It is found that the force measured at a distance of 1.4 m from the negative ion source correlates well with the momentum flux that is calculated from the ion energy and the averaged extracted ion current density.

Schematic of the force-probe diagnostic for momentum-flux measurements in the negative hydrogenion beam at the BATMAN facility. A water-cooled shield with a 5 mm aperture limits the beam spot on an L-shaped tungsten target mounted on an interferometric cantilever probe, enabling charge-independent local flux determination 1.4m downstream of the source

提出了一种测定中性束注入器(NBI)束流中粒子通量密度的新方法。该方法使用一个力探针来测量从束粒子到小目标的动量转移,并已在MPI Garching的BATMAN实验设施中应用。本报告中的实验是在未中和的负离子束流中进行的。在距离负离子源1.4 m处测得的力与由离子能量和提取的平均离子电流密度计算得到的动量通量具有良好的相关性。在BATMAN设施中用于负氢离子束动量通量测量的力探针诊断示意图。一个孔径为5mm的水冷罩将光束光斑限制在安装在干涉悬臂式探头上的l形钨靶上,从而能够在源下游1.4m处进行与电荷无关的局部通量测定
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引用次数: 0
The measurement problem in liquid NMR quantum computers 液体核磁共振量子计算机中的测量问题
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-10-06 DOI: 10.1140/epjd/s10053-025-01072-0
O. Jalili, M. Heidari Adl

With the quantum state diffusion measurement theory (QSD), the measurement problem in liquid nuclear magnetic resonance (NMR) quantum computers was addressed and then it was shown that due to stochastical fluctuations, the measured magnetic moment value is comparable to noise for long times. Therefore, we suggested that the measurement time should be short to distinguish signal from noise.

QSD in NMR quantum computers.

利用量子态扩散测量理论(QSD)解决了液体核磁共振(NMR)量子计算机中的测量问题,并证明了由于随机波动,测量的磁矩值在很长时间内与噪声相当。因此,我们建议测量时间应短,以区分信号和噪声。核磁共振量子计算机中的QSD。
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引用次数: 0
Interaction of 25 eV electrons with DNA constituents: XPS analysis of calf thymus DNA, nucleosides, and nucleobases 25 eV电子与DNA成分的相互作用:小牛胸腺DNA、核苷和核碱基的XPS分析
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-10-06 DOI: 10.1140/epjd/s10053-025-01068-w
João Pereira-da-Silva, Hao Yu, Bo-An Chen, Pitambar Sapkota, Filipe Ferreira da Silva, Sylwia Ptasińska

Understanding the interactions of secondary electrons generated by ionizing radiation provides a fundamental basis for developing strategies in cancer therapy. In this study, we investigated the interactions of 25 eV low-energy electrons (LEEs) with calf thymus DNA and its constituents, four types of nucleosides and nucleobases, using X-ray photoelectron spectroscopy (XPS). Based on the acquisition and analysis of core-level spectra (O 1s, C 1s, N 1s, and P 2p) in DNA, structural changes induced by 25 eV electrons suggest potential site- and base-specific selectivity. These changes may involve hydroxyl (C–OH) group release from the sugar moiety, cleavage of C–N bonds (likely corresponding to N-glycosidic linkages), and phosphate backbone damage in calf thymus DNA. Among the four nucleosides, thymidine and guanosine showed more evident structural modifications, while cytidine and adenosine were relatively stable. In addition, nucleosides displayed greater susceptibility to LEE-induced structural changes than their corresponding nucleobases. This study reveals the selective damage mechanisms of LEEs on various DNA constituents, which may provide mechanistic insights for future developments in precision cancer therapy based on molecular-level damage.

Graphical abstract

了解电离辐射产生的二次电子的相互作用为制定癌症治疗策略提供了基础。本研究利用x射线光电子能谱(XPS)研究了25 eV低能电子(LEEs)与小牛胸腺DNA及其组分(4种核苷和核碱基)的相互作用。基于DNA核能级光谱(O 1s, C 1s, N 1s和P 2p)的采集和分析,25 eV电子诱导的结构变化表明潜在的位点和碱基特异性选择性。这些变化可能涉及羟基(C-OH)基团从糖部分释放,C-N键的断裂(可能对应于n -糖苷键),以及小牛胸腺DNA中磷酸盐骨干的损伤。四种核苷中胸苷和鸟苷的结构变化较为明显,胞苷和腺苷的结构变化相对稳定。此外,核苷比其相应的核碱基更容易受到lee诱导的结构变化的影响。该研究揭示了LEEs对不同DNA成分的选择性损伤机制,为未来基于分子水平损伤的精准癌症治疗提供了机制见解。图形抽象
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引用次数: 0
Highly accurate calculation of the hyperpolarizabilities of hydrogenic atoms interacting with screened Coulomb potentials: a variation–perturbation approach 与筛选库仑势相互作用的氢原子超极化率的高度精确计算:一种变差摄动方法
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-10-06 DOI: 10.1140/epjd/s10053-025-01073-z
Santu Ghosh, Arijit Ghoshal

Variational expressions for functionals yielding the second-order and fourth-order corrections to the nondegenerate eigenenergies of a Hamiltonian subject to a given perturbation have been derived. Discrete basis sets consisting of the suitably chosen eigenfunctions of the unperturbed Hamiltonian along with a nonlinear variational parameter can be used to evaluate the stationary functional quite accurately. The method has been applied conveniently to calculate the dipole hyperpolarizabilities of the hydrogenic atoms interacting with screened Coulomb potentials (SCP) quite accurately. Three SCPs are considered, namely the static screened Coulomb potential, the exponential cosine screened Coulomb potential and the generalized exponential cosine screened Coulomb potential. It is found that a basis set consisting of 20 eigenfunctions of the p-states of the hydrogenic atoms yields stationary functional corresponding to the second-order correction to the energy, whereas a basis set consisting of 20 d-state eigenfunctions and 19 s-state eigenfunctions of the hydrogenic atoms produces stationary functional corresponding to the fourth-order correction to the energy. Moreover, the stationary values of the functionals are highly accurate (up to 14th place of decimal) and converge rapidly with the increase in the number of terms in the basis sets.

对哈密顿函数在给定扰动下的非简并特征能给出二阶和四阶修正的泛函变分表达式。由适当选择的无扰动哈密顿函数的特征函数和非线性变分参数组成的离散基集可以相当精确地计算平稳泛函。该方法可方便地计算出与筛选库仑势相互作用的氢原子的偶极子超极化率。考虑了静态屏蔽库仑势、指数余弦屏蔽库仑势和广义指数余弦屏蔽库仑势这三种电位。研究发现,由20个氢原子p态本征函数组成的基集产生的平稳泛函对应于能量的二阶修正,而由20个氢原子d态本征函数和19个氢原子s态本征函数组成的基集产生的平稳泛函对应于能量的四阶修正。此外,函数的平稳值具有很高的精度(可达小数点后14位),并且随着基集中项数的增加而迅速收敛。
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引用次数: 0
The effect of space restriction on the bonding and vibrational properties of H(_{2}^{+}) molecular ion 空间限制对H (_{2}^{+})分子离子成键和振动特性的影响
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-09-30 DOI: 10.1140/epjd/s10053-025-01062-2
Claude Le Sech, Arup Banerjee

When the space surrounding an atom or molecule is restricted, its electron density is modified compared to its unrestricted counterpart, which further alters its physical and chemical properties. To model the effect of space restriction, or confinement, on atoms and molecules, often the hard-boundary condition is employed to solve the corresponding Schrödinger equation. In the present work, we analyze the modifications in a chemical bond when the space surrounding the molecule is restricted such that some part of the space is forbidden to the electrons. To this end, we choose the simplest hydrogen molecular ion H(_{2}^{+}), in the presence of an external hard-sphere simulating the restriction of space available to the electrons due to Pauli exclusion by an atom close to the molecule. The hard-sphere is moved along the molecular axis and the axis transverse to it to study the changes in the ground-state energy, stretching frequency, kinetic, and potential energies of an H(_{2}^{+}) molecule. For this purpose, we employ a variational approach using a suitably constructed energy estimator that goes beyond the Born–Oppenheimer approximation. We find that as the sphere moves closer to the molecule along the molecular axis, the ground-state energy and the vibrational frequencies get enhanced. On the other hand, for the same case, the potential energy decreases, and the kinetic energy increases. When the sphere moves along the axis transverse to the molecular axis, the changes in the energy and vibrational frequencies show similar trends; however, the magnitude of the changes is significantly smaller than in the corresponding molecular axis case. For the transverse case, both potential and kinetic energies get enhanced marginally. These results demonstrate that the axial approach of the hard surface is more efficient in inducing a bond breaking of the H(_{2}^{+}) molecular ion. The shift of the electron bond by the external sphere explains these results.

当一个原子或分子周围的空间受到限制时,它的电子密度与不受限制的电子密度相比会发生改变,这进一步改变了它的物理和化学性质。为了模拟空间限制或约束对原子和分子的影响,通常采用硬边界条件来求解相应的Schrödinger方程。在目前的工作中,我们分析了当分子周围的空间受到限制,使得某些空间禁止电子进入时,化学键中的修饰。为此,我们选择了最简单的氢分子离子H (_{2}^{+}),在外部硬球的存在下,模拟了由于泡利不相容而导致的电子可用空间的限制。将硬球沿分子轴及其横向轴移动,研究H (_{2}^{+})分子的基态能量、拉伸频率、动能和势能的变化。为此,我们采用了一种变分方法,使用了一个适当构造的能量估计器,超出了Born-Oppenheimer近似。我们发现,当球沿分子轴向分子靠近时,基态能量和振动频率得到增强。另一方面,对于同样的情况,势能减小,动能增大。当球沿分子轴横向运动时,能量和振动频率的变化也表现出类似的趋势;然而,变化幅度明显小于相应的分子轴情况。在横向情况下,势能和动能都略微增大。这些结果表明,硬表面的轴向方法更有效地诱导H (_{2}^{+})分子离子的键断裂。外部球体对电子键的移动解释了这些结果。
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引用次数: 0
Density matrix analysis of systems with periodic Hamiltonians 具有周期哈密顿量系统的密度矩阵分析
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-09-29 DOI: 10.1140/epjd/s10053-025-01070-2
Soham Sen, Manjari Dutta, Sunandan Gangopadhyay

In this work, we consider simple systems that are governed by Hamiltonians with time periodicity. Our analysis is mainly focused on the density matrix approach and aims to solve the von Neumann equation of motion from which one can extract the state of the system when the system is in a pure state. We start our analysis with the standard Rabi-oscillation problem. We consider a density matrix corresponding to the entire model system and solve the von Neumann equation of motion. We have then made use of the Lewis-Reisenfeld invariant approach and arrived at the exact same result, which implies that the density matrix of the system can indeed be identified with the Lewis invariant. Then, we consider a two-level system with a constant magnetic field in the z-direction and a time-dependent magnetic field in the x-direction. We solve the von Neumann equation of motion for this system and calculate the various coherence measures, and plot them to investigate the time dependence and reliability of different coherence measures.

Correspondence between the density operator and the Lewis invariant operator of the system

在这项工作中,我们考虑由具有时间周期性的哈密顿量控制的简单系统。我们的分析主要集中在密度矩阵方法上,旨在求解冯·诺伊曼运动方程,从中可以提取系统处于纯态时的状态。我们从标准拉比振荡问题开始分析。我们考虑一个与整个模型系统相对应的密度矩阵,并求解了运动的冯·诺伊曼方程。然后我们利用Lewis- reisenfeld不变量方法得到了完全相同的结果,这意味着系统的密度矩阵确实可以用Lewis不变量来标识。然后,我们考虑一个两能级系统,在z方向上具有恒定磁场,在x方向上具有随时间变化的磁场。我们求解了该系统的von Neumann运动方程,计算了各种相干测度,并绘制了它们的图,以研究不同相干测度的时间依赖性和可靠性。系统的密度算子与路易斯不变算子的对应关系
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引用次数: 0
Elastic and charge transfer cross sections for low to ultralow (textrm{H}(1s)+textrm{H} ^{+}) collisions: quantal and semiclassical calculations 低至超低(textrm{H}(1s)+textrm{H} ^{+})碰撞的弹性和电荷转移截面:量子和半经典计算
IF 1.5 4区 物理与天体物理 Q3 OPTICS Pub Date : 2025-09-29 DOI: 10.1140/epjd/s10053-025-01059-x
Mykhaylo Khoma

The elastic scattering and resonant charge transfer differential and integral cross sections in (textrm{H}(1s) + mathrm{H^+}) collisions are computed for the center-of-mass energy range of (10^{-10}-10) eV. Fully quantal and semiclassical approaches are utilized in these calculations. The reliability of the semiclassical approximation for very low collision energies is discussed. The results are compared with available data from the literature.

在(10^{-10}-10) eV的质心能量范围内,计算了(textrm{H}(1s) + mathrm{H^+})碰撞中的弹性散射和共振电荷转移微分截面和积分截面。在这些计算中使用了全量子和半经典方法。讨论了在极低碰撞能量条件下半经典近似的可靠性。结果与文献中的现有数据进行了比较。
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引用次数: 0
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The European Physical Journal D
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