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Crystallization in mass-asymmetric electron-hole bilayers P. 1 1,2 Ludwig , A. 1,3 Filinov , Yu. E. 3 Lozovik , H. 2 Stolz and M. Institute of Theoretical Physics and Astrophysics, CAU-Kiel, Leibnizstrasse 15, D-24098, Germany 2 Institute of Physics, University of Rostock, Universitätsplatz 3, D-18051, Germany 3 Institute of Spectroscopy RAS, Moscow region, Troitsk, 142190, Russia 1 Holes and electrons in a bilayer system with d=20aB Abstract M=5 We analyze hole crystallization [1] in an electron-hole bilayer system and specifically study the effect of the hole to electron mass ratio M. Varying M=mh/me in the range 1 ≤ M ≤ 100 at a fixed layer separation d, we demonstrate that the hole behavior can be tuned from a delocalized (liquid-like) to a localized (crystal-like) state, while the electrons remain delocalized (me is fixed). As was recently demonstrated [1] in bulk systems holes undergo a crystallization transition if the mass ratio exceeds a critical value of Mcr ≈ 83. Here we extend this analysis to bilayer systems and demonstrate that the critical mass ratio can be drastically reduced by properly choosing the layer separation. The complicated interplay between Coulomb correlations and quantum effects of both, electrons and holes, is fully taken into account by performing first principle path integral Monte Carlo simulations. We present results for two types of e-h bilayers: a) a mesoscopic system of Ne=Nh=36 electron and holes in a parabolic trap and b) for a macroscopic system with similar density. Model and parameters =H e H h −∑ H N ∑ i=1 j=i1 ei e j r i −r j 2 z i −z j N e h e h= ∑ , H 2 i=1 ∗ me h 2 2 ℏ2 2 − ∇r e h r i , ∗ 2 2m e h i where the electrons (e) are confined to the plane z=0 and the holes (h) to the plane z=d; also ri and rj are the inplane 2D radius vectors describing the particle coordinates in each layer. We assume that the electrons and holes are in a thermal equilibrium and cooled down by using, e.g. 3He/4He dilution refrigeration, to a temperature of kBT = 1/3000 Ha. At these low temperatures thermal fluctuations are negligible and the system is practically in the ground state. The applied path integral Monte Carlo technique is discussed in Ref. [2] and references therein. System of units: Typical configurations of holes (blue points) and electrons (red dots) in the bilayer without statistical averaging. Shown is the PIMC representation of quantum particles. Each particle is presented by a set of 256 dots. The electrons are completely delocalized. First two rows: 36 electrons and holes in the harmonic trap with λ=5 (upper panel) and λ=10.5 (second panel). Due to the confinement symmetry, for M=100 the holes are arranged in 3 concentric shells populated with 16, 12, 7 and a single particle in the center. λ=10.5 (meso) Row 3: Macroscopic bilayer with Ne = Nh = 64 electrons and holes in the simulation cell with periodic boundary conditions. The density matches that in the mesoscopic system of the second raw. There are structural defects as the triangular lattice is not uniform.. The electron-hole mass ratio M=me/mh drives the crystallization: - the electrons are distributed almost continuously in all cases - the holes become localized for M≥20 (λ=5) and M≥5 (λ=10.5), respectively. Macroscopic system The main difference between the mesoscopic system with a parabolic in-plane confinement and an infinite system are finite size effects which are related to the rotational symmetry instead of translational symmetry. In contrast to the trapped system, in the macroscopic system the average particle density is constant over the entire system. We considered Ne=Nh=64 electrons and holes in a simulation cell of the size {Lx × Ly} = {152.37aB × 131.956aB} with periodic boundary conditions. This corresponds to a density parameter rs=<r>/aB=10. The density was chosen to be comparable to the average density in the finite system for the case of coupling parameter λ = 10.5. As in the mesoscopic system, for all cases the electrons are completely delocalized. In contrast, the hole localization increases from M = 5 to M = 100 (cf. plots of the ghh function of the finite and infinite system). energy scale: E/Ha, 1 Ha = e2/ε aB =11.5meV (GaAs); 53.9meV (ZnSe) length scale: r/aB, 1 aB= ћ2ε/mee2 =9.98nm (GaAs); 3.07nm (ZnSe) Hole-hole (top) and electron-hole (bottom) pair distribution functions for the macroscopic bilayer with Ne=Nh=64 for the mass ratios M = 1, 3, 4, 5, 10, 20 (the amplitudes increase with increasing M). Simulated temperature: kBT/Ha = 1/3000 Ha = 44.37mK (GaAs); 208.6mK (ZnSe) 3 M=100 λ=5 (meso) 4 We approximate two coupled quantum wells by a model of two vertically separated 2D layers populated with Ne electrons and Nh holes (we consider the case Ne = Nh = N/2). The charges interact via the Coulomb potential. For the chosen interlayer distance d = 20aB our system represents essentialy a 3D structure, as the intralayer and interlayer correlations are on the same length and energy scales. The underlying Hamiltonian is well defined and is of practical importance for semiconductor heterostructures N M=20 λ=10.5 (macro) [1] M. Bonitz, V.S. Filinov, V.E. Fortov, P.R. Levashov, and H. Fehske, Phys. Rev. Lett. 95, 235006 (2005) and J. Phys. A: Math. Gen. 39, 4717 (2006); Phys. Rev. Focus, December 2 2005 [2] P. Ludwig, A. Filinov, Yu. Lozovik, H. Stolz, and M. Bonitz, Contrib. Plasma Phys. (2007) 2 1 Bonitz For M ≥ 4 we observe clear oscillations in ghh, typical for the solid phase. Even the third and fourth peaks are well resolved. For M = 3 and below the PDF shows liquid-like features. The third peak is strongly suppressed. Mesoscopic system We consider a bilayer system with Ne=Nh=36 electrons and holes. Control parameters: - harmonic trap frequency meωe2=mhωh2 - coupling strength λ = (e2/ε l0)/(ћωe) = l0/aB with l02=ћ/meωe Also, for M ≥ 4 a minimum of geh at zero distance appears and the function exhibits oscillations. With formation of the hole crystal the electron density becomes slightly modulated with alternating location of maxima and minima of ghh and geh. I.e., the electron density is amplified inbetween the holes. We analyzed two different densities, given by λ=5 and λ=10.5 which corresponds to the average densities (in a single layer) for GaAs nλ=5=9.4·109/cm2 and nλ=10.5=2.0·109/cm2, and for ZnSe nλ=5=9.9·1010/cm2 and nλ=10.5= 2.2·1010/cm2. Changing the mass ratio from M = 1 to 100 the holes exhibit a transition from quantum liquid with wave function overlap to a spatially ordered structure, while the electrons stay always in a quantum fluid state with a slightly modulated homogeneous density (see Fig. below). The classical Coulomb coupling parameter Γ=e2/(<r> kBT) (the ratio of mean correlation and kinetic energy) for the holes with M=100 equals Γλ=5 = 345 and Γλ=10.5 = 158 , which is above the critical value for the macroscopic (one-component plasma) crystallization Γcr =137. Radial, nh, and pair, ghh, distribution for the holes and the coupling strengths λ=5 and five mass ratios. The average density is highest in the center and decreases towards the cluster surface. localization transition: ur=0.15 With increasing M the holehole correlations lead to formation of distinct shells. The peak of ghh stays unchanged due to the conditions meωe2=mhωh2, hence the frequency scales as ωh~M-1/2. Hole-hole (upper fig.) and electron-hole (lower fig.) pair distribution functions (PDF) for the mesoscopic bilayer with Ne = Nh = 36 and λ=10.5. The distributions are normalized to the corresponding PDF for the case M = 1 to eliminate the effect of the decay of the average density in the finite system. The electrons and holes on the average are aligned vertically. Compare the positons of the peaks of ghh and geh. The plot includes distances up to two times the radius which causes the increase of the PDF for large distances. We use Lindemann criteria to identify the critical mass ratio Mcr when the holes crystallize 2r N N 2 u = 2= 〈r ij2 〉 / 〈 r ij 〉 2−1 ∑ ∑ r 0 N N −1 i =1 j =i1 2 r The critical values are Mcr(λ=5) ≈ 5 and Mcr(λ=10.5) ≈ 2.8, in the mesoscopic system, and Mcr(rs=10) ≈ 3.1, in the macroscopic system. Decay of the amplitude of the maxima and minima of |ghh − 1| in the macroscopic system for different mass ratios. The change from an exponential (for M≤3) to a power law decay (for M≥4) signals a Kosterlitz-Thouless-like transition. Analysis of the dominant effects: i) Mcr depends on density, it decreases when the coupling strength λ increases. ii) There is good agreement between the critical mass ratios of the mesoscopic and the macroscopic system (within 10%). iii) The critical values are much smaller than the value of Mcr ≈ 80 in a 3D bulk system [1] which underlines the remarkable additional control of physical behaviors existing in a bilayer system by a variation of the layer separation d. iv) The presence of the electron layer leads to stabilization of the „ordered state“ of the holes. It is expected that further reduction of d will allow to further reduce Mcr and to increase the maximum density of the hole crystal to values below rs(h) = 20.