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超强激光场中分子团簇的电子与核动力学。II. 纳米等离子体的电子动力学与外层电离

Electron and nuclear dynamics of molecular clusters in ultraintense laser fields. II. Electron dynamics and outer ionization of the nanoplasma.

作者信息

Last Isidore, Jortner Joshua

机构信息

School of Chemistry, Tel Aviv University, Ramat Aviv, 69978 Tel Aviv, Israel.

出版信息

J Chem Phys. 2004 Jan 15;120(3):1348-60. doi: 10.1063/1.1630308.

Abstract

We explore electron dynamics in molecular (CD4)(1061) clusters and elemental Xen (n=249-2171) clusters, responding to ultraintense (intensity I=10(16)-10(19) W cm(-2)) laser fields. Molecular dynamics simulations (including magnetic field and relativistic effects) and analyses of high-energy electron dynamics and nuclear ion dynamics in a cluster interacting with a Gaussian shaped laser field (frequency 0.35 fs(-1), photon energy 1.44 eV, phase 0, temporal width 25 fs) elucidated the time dependence of inner ionization, the formation of a nanoplasma of unbound electrons within the cluster or its vicinity, and of outer ionization. We determined the cluster size and the laser intensity dependence of these three sequential-parallel electronic processes. The characteristic times for cluster inner ionization (tau(ii)) and for outer ionization (tau(oi)) fall in the femtosecond time domain, i.e., tau(ii)=2-9 fs and tau(oi)=4-15 fs for (CD4)(1061), tau(ii)=7-30 fs and tau(oi)=5-13 fs for Xe(n) (n=479,1061), with both tau(ii) and tau(oi) decreasing with increasing I, in accord with the barrier suppression ionization mechanism for inner ionization of the constituents and the cluster barrier suppression ionization mechanism for outer ionization. The positive delay times Deltatau(OI) between outer and inner ionization (e.g., Deltatau(OI)=6.5 fs for Xen at I=10(16) W cm(-2) and Deltatau(OI)=0.2 fs for (CD4)(1061) at I=10(19) W cm(-2)) demonstrate that the outer/inner ionization processes are sequential. For (CD4)(1061), tau(ii)<tau(oi), as appropriate for sequential outer/inner ionization dynamics, while for Xen clusters tau(ii)>tau(oi), reflecting on the energetic hierarchy in the ionization of the Xe atoms. Quasiresonance contributions to the outer ionization of the nanoplasma were established, as manifested in the temporal oscillations in the inner/outer ionization levels, and in the center of mass of the nanoplasma electrons. The formation characteristics, dynamics, and response of the nanoplasma in molecular or elemental clusters were addressed. The nanoplasma is positively charged, with a high-average electron density [rho(P)=(2-3)10(22) cm(-3)], being characterized by high-average electron energies epsilon(av) (e.g., in Xe(1061) clusters epsilon(av)=54 eV at I=10(16) W cm(-2) and epsilon(av)=0.56-0.37 keV at I=10(18) W cm(-2), with epsilon(av) proportional, variant I(1/2)). Beyond the cluster boundary the average electron energy markedly increases, reaching electron energies in the range of 1.2-40 keV for outer ionization of Xe(n) (n=249-2171) clusters. The nanoplasma exhibits spatial inhomogeneity and angular anisotropy induced by the laser field. Femtosecond time scales are predicted for the nanoplasma production (rise times 7-3 fs), for the decay (decay times approximately 5 fs), and for the persistence time (30-10 fs) of a transient nanoplasma at I=10(17)-10(18) W cm(-2). At lower intensities of I=10(16) W cm(-2) a persistent nanoplasma with a "long" lifetime of > 50 fs will prevail.

摘要

我们研究了分子(CD4)(1061)团簇和元素氙(Xe)(n = 249 - 2171)团簇中的电子动力学,这些团簇对超强(强度I = 10(16) - 10(19) W cm(-2))激光场做出响应。通过分子动力学模拟(包括磁场和相对论效应)以及对与高斯形状激光场(频率0.35 fs(-1),光子能量1.44 eV,相位0,时间宽度25 fs)相互作用的团簇中的高能电子动力学和核离子动力学进行分析,阐明了内电离的时间依赖性、团簇内部或其附近未束缚电子的纳米等离子体的形成以及外电离。我们确定了这三个相继并行电子过程的团簇尺寸和激光强度依赖性。团簇内电离(tau(ii))和外电离(tau(oi))的特征时间落在飞秒时域内,即对于(CD4)(1061),tau(ii)=2 - 9 fs且tau(oi)=4 - 15 fs;对于Xe(n)(n = 479,1061),tau(ii)=7 - 30 fs且tau(oi)=5 - 13 fs,tau(ii)和tau(oi)均随I的增加而减小,这符合组分内电离的势垒抑制电离机制和外电离的团簇势垒抑制电离机制。外电离和内电离之间的正延迟时间Deltatau(OI)(例如,在I = 10(16) W cm(-2)时,Xe的Deltatau(OI)=6.5 fs;在I = 10(19) W cm(-2)时,(CD4)(1061)的Deltatau(OI)=0.2 fs)表明外/内电离过程是相继发生的。对于(CD4)(1061),tau(ii)<tau(oi),这适合相继的外/内电离动力学,而对于Xe团簇,tau(ii)>tau(oi),反映了Xe原子电离中的能量层级。确定了纳米等离子体外电离的准共振贡献,这表现为内/外电离水平以及纳米等离子体电子质心的时间振荡。研究了分子或元素团簇中纳米等离子体的形成特征、动力学和响应。纳米等离子体带正电,具有高平均电子密度[rho(P)=(2 - 3)10(22) cm(-3)],其特征是具有高平均电子能量epsilon(av)(例如,在I = 10(16) W cm(-2)时,Xe(1061)团簇中的epsilon(av)=54 eV;在I = 10(18) W cm(-2)时,epsilon(av)=0.56 - 0.37 keV,且epsilon(av)与I(1/2)成正比、变化)。在团簇边界之外,平均电子能量显著增加,对于Xe(n)(n = 249 - 2171)团簇的外电离,电子能量达到1.2 - 40 keV范围。纳米等离子体表现出由激光场引起的空间不均匀性和角各向异性。预测了在I = 10(17) - 10(18) W cm(-2)时纳米等离子体产生的飞秒时间尺度(上升时间7 - 3 fs)、衰变(衰变时间约5 fs)以及瞬态纳米等离子体的持续时间(30 - 10 fs)。在较低强度I = 10(16) W cm(-2)时,将存在寿命大于50 fs的持久纳米等离子体。

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