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Electron bubbles in helium clusters.I.Structure and energetics

机译:氦团簇中的电子气泡I.结构与能量学

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In this paper we present a theoretical study of the structure,energetics,potential energy surfaces,and energetic stability of excess electron bubbles in (~4He)_N (N=6500-10~6) clusters.The subsystem of the helium atoms was treated by the density functional method.The density profile was specified by a void (i.e.,an empty bubble) at the cluster center,a rising profile towards a constant interior value (described by a power exponential),and a decreasing profile near the cluster surface (described in terms of a Gudermannian function).The cluster surface density profile width (approx 6 A) weakly depends on the bubble radius R_b,while the interior surface profile widths (approx 4-8 A) increase with increasing R_b.The cluster deformation energy E_d accompanying the bubble formation originates from the bubble surface energy,the exterior cluster surface energy change,and the energy increase due to intracluster density changes,with the latter term providing the dominant contribution for N= 6500-2 X 10~5.The excess electron energy E_e was calculated at a fixed nuclear configuration using a pseudopotential method,with an effective (nonlocal) potential,which incorporates repulsion and polarization effects.Concurrently,the energy V_0 of the quasi-free-electron within the deformed cluster was calculated.The total electron bubble energies E_t=E_e+E_d,which represent the energetic configurational diagrams of E_t vs R_b,(at fixed N,provide the equilibrium bubble radii R_b~c and the corresponding total equilibrium energies E_t~e,with E_t~e(R_e) decreasing (increasing) with increasing N (i.e.,at N=6500,R_e=13.5 A and E_t~e=0.86 eV,while at N=1.8 X 10~5,R_e=16.6 A and E_t~e=0.39 eV).The cluster size dependence of the energy gap (V_0 -E_t~e) allows for the estimate of the minimal (~4He)_N,cluster size of N approx= 5200 for which the electron bubble is energetically stable.
机译:本文对(〜4He)_N(N = 6500-10〜6)团簇中多余电子气泡的结构,能量学,势能面和能量稳定性进行了理论研究。对氦原子的子系统进行了处理密度分布由簇中心的空隙(即空泡),朝向恒定内部值的升高分布(由幂指数描述)和在簇表面附近的降低分布指定(用Gudermannian函数描述)。团簇表面密度轮廓宽度(约6 A)弱依赖于气泡半径R_b,而内表面轮廓宽度(约4-8 A)随R_b的增加而增加。伴随气泡形成的能量E_d来源于气泡表面能,外部簇表面能的变化以及由于团簇内密度变化而增加的能量,后一项在N = 6500时起主要作用-2 X 10〜5。在固定核构型下使用伪电势方法计算了多余的电子能量E_e,其中具有有效(非局部)电势,其中包含了排斥和极化效应。同时,准自由电子的能量V_0计算了变形簇中的电子。总电子气泡能量E_t = E_e + E_d,代表了E_t与R_b的能量结构图(在固定N下,提供了平衡气泡半径R_b〜c和相应的总平衡能量E_t 〜e,E_t〜e(R_e)随着N的增加而减小(增加)(即,在N = 6500,R_e = 13.5 A,E_t〜e = 0.86 eV,而在N = 1.8 X 10〜5,R_e = 16.6时) A和E_t〜e = 0.39 eV)。能隙的簇大小相关性(V_0 -E_t〜e)允许估计电子气泡的最小(〜4He)_N,N的簇大小约为5200能量稳定。

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