Polaron Effects on The Optical Absorption Coefficients in A Cylindrical ZnS/CdSe Core-Shell Quantum Dot

CHEN Zhi-hong, LI Qian-guang, YI Xu-nong, YU Hua-qing, XIONG Liang-bin

(SchoolofPhysicsandElectronic-informationEngineering,HubeiEngineeringUniversity,Xiaogan432000,China)

Polaron Effects on The Optical Absorption Coefficients in A Cylindrical ZnS/CdSe Core-Shell Quantum Dot

CHEN Zhi-hong, LI Qian-guang*, YI Xu-nong, YU Hua-qing, XIONG Liang-bin

(SchoolofPhysicsandElectronic-informationEngineering,HubeiEngineeringUniversity,Xiaogan432000,China)

The polaron effects on the linear and nonlinear optical absorption coefficients are investigated theoretically for electrons confined in a core-shell quantum dot. The interactions of electrons with the confined longitudinal optical (LO) and the interface optical (IO) phonon modes in the core-shell system are investigated. An analytic formula for the optical absorption is derived with compact-density-matrix approach and iterative method. The optical absorption coefficients in a ZnS/CdSe core-shell quantum dot (QD) are calculated numerically for different pump photon energies, incident optical intensities and relaxation times. Results show that the optical absorption coefficients are dependent on the photon energy and relaxation time dramatically. Moreover, when the electron-LO phonon interaction is considered, the optical absorption coefficient is enhanced more than 2 times.

polarons; core-shell quantum dot; optical absorption

1 Introduction

In recent years, much attention has been focused on the nonlinear optical properties of low-dimensional semiconductor structures[1-3], such as semiconductor quantum dot (QD). The quantum confinement of electrons in all three dimensions in QDs can result in the formation of discrete electron energy levels and the generation of a large number of linear and nonlinear optical phenomena compared with bulk semiconductors[4]. Recently，core-shell QDs with spherical symmetry have been the object of detailed experimental and theoretical investigations[5-6]. A core-shell QD is a nanometer structure with a “core” in its middle. Since it has considerable exceptional optical properties, core-shell QDs have attracted great interest in the physics and technological applications[7-8]. Hence， it is believed that a fundamental study on the optical properties of a core-shell QD is very important[9].

Among the electronic and optical properties in low dimensional structures, nonlinear optical properties are widely investigated, especially when optical absorption coefficients appeal to many researchers[10-13]. Zhangetal. studied the optical absorption coefficients and the variation of refractive index in parabolic quantum dots[10]. Yusuf Yakaretal. investigated the linear and nonlinear optical absorption coefficients of a spherical quantum dot with parabolic potential[11]. Yesilguletal. researched the effect of intense high-frequency laser field on the linear and nonlinear intersubband optical absorption coefficients and refractive index changes in a parabolic quantum well, considering applied electric field[12]. Gambhiretal. reported linear and nonlinear optical absorption coefficients and the variation of refractive index associated with intersubband transitions in a quantum disk with flat cylindrical geometry[14]. Their studies are concerned about optical absorption coefficients, and found that the optical absorption coefficients are strongly influenced by the impurity, incident optical intensity, relaxation time, and parabolic potential.

Meanwhile, many researchers have concentrated their attention on the effects of the electron-optical phonon interaction, especially in low-dimensional quantum systems[15-16]. Guoetal. reported the polaron effects on the third-harmonic generation for electrons confined in asymmetrical semi-exponential quantum wells[15]. They found that the third-harmonic generation is obviously increased when the electron-LO-interaction is taken into account. Mouetal. reported polaron effects on the linear and nonlinear intersubband optical absorption coefficients in quantum wells with asymmetrical semi-exponential potential[16]. The results of calculation show that optical absorption is enhanced when effects of polaron are considered. All research results have revealed that the electron-phonon interaction becomes more and more important in electronic properties and optical properties with the decreasing of the dimension.

However， there are few studies treating the electron-phonon interaction on the optical absorption in a core-shell quantum dot. Theoretically, this paper attempts to examine the linear and nonlinear optical absorption coefficients in a core-shell quantum dot taking polaron effects into account. The analytical expressions of the optical absorption coefficients are to be obtained by using density-matrix method and iterative method. In Section 3, the numerical results and some discussions are to be presented. A conclusion is drawn in Section 4.

2 Theory

2.1 Electron, Phonon and Electron-phonon Interaction Hamiltonian

The model considered in the paper is a suppositional core-shell cylindrical quantum dot with a centric barrier (ZnS) and a shell layer (CdSe), the outer space is filled with nonpolar medium: water, which can be treated as an infinite barrier, and the electromagnetic fieldE(ω)isparalleltotheZ-axis(shown in Fig.1 ).distheheightofthecylinder,andR1andR2aretheinnerandouterradii.

Undertheframeworkofeffective-massapproximation,theHamiltonian[17]ofthesystemcanbewrittenas

(1)

ThefirstterminEq. (1)istheHamiltonianofelectronHe, it is given by

(2)

Fig.1Modelofasuppositionalcore-shellcylindricalquantumdots

ThesecondtermisthefreephononHamiltonian:

(3)

The last term of Eq. (1) stands for the electron-phonon interaction Hamiltonian:

(4)

He-LO1denotes the Hamiltonian of the electron interaction with LO phonon in the core[18]:

(5)

Jm(x) is the Bessel function of the first kind.xmlis themth zero ofJm(x).

Correspondingly,He-LO2is the Hamiltonian of the electron interaction with LO phonon in the shell[18]:

(6)

Tml(amlr/R1)satisfies the boundary conditions:

(7)

In Eq.(4), the last termHe-IOis the Hamiltonian of the electron interaction with IO phonon[18]:

(8)

2.2 Linear and Nonlinear Absorption Coefficients

The wave function of an electron in the core-shell quantum dot can be resolved from the Schr?dinger equation of an electron[19]:

(9)

It is noted that the wave function above must satisfy the normalization condition. Besides, they must satisfy the boundary condition:

(10)

(11)

(12)

whereR<,R>standforthewavefunctionRfor the cases ofrR1.

Weassumethatthesystemwereinlowtemperature(T→0),sotheinitialstatewouldbethephononvacuumstate.Inthecourseofphonontransition,onlyone-phononabsorption(emission)isconsidered.Undertheframeworkofperturbationtheory,thesystemwavefunctioncanbewrittenas

whereε=?ωLOor ?ωIO.

By using the compact density-matrix approach and iterative method, the optical absorption coefficients can be obtained. The electronic polarizationP(t) is formulated as

(14)

In our work, the optical absorption coefficients[10]can be expressed by

(15)

(16)

Thetotalabsorptioncoefficientisobtainedby

(17)

3 ResultsandDiscussion

TheopticalabsorptioncoefficientsinaZnS/CdSecore-shellcylindricalquantumdotarecalculatednumericallywithequation(17).TheparametersofZnSandCdSearelistedinTab.1[20].

Tab.1 Material parameters (m0is the rest electron mass) used in the calculation

Materialm*/m0?ωLO/meV?ωTO/meVε0ε￥ZnS0.2843.633.678.15.14CdSe0.1326.4120.839.566.23

The conduction band discontinuity and electron density areVc=0.9 eV andN=5×1024m-3respectively in all calculations.

In Fig.2, the linear, third-order nonlinear and total optical absorption coefficients are plotted as a function of the photon energy ?ω.TheincidentopticalintensityisI=0.5×1010W/m2,andtheparametersofthecore-shellcylindricalQDareR1=4.5 nm,R2=7.5 nm andd=4.0 nm. Two cases are analyzed using: electron-LO-phonon interaction effects and without electron-phonon interaction effects, which are illustrated by the dotted line and solid line, respectively. Judging from Fig.2, we can see that it is obvious that the large linear absorption coefficientα(1)ispositivewhereasthethird-ordernonlinearopticalabsorptioncoefficientα(3)isnegative.Sothetotalopticalabsorptioncoefficientαissignificantlyreducedbytheα(3)contribution.Therefore,thethird-ordernonlinearopticalabsorptioncoefficientα(3)shouldbeconsideredwhentheincidentopticalintensityIiscomparativelystrong,whichcaninducenonlinearabsorption.However,whenweconsidertheelectron-LOphononinteractioneffect,theopticalabsorptioncoefficientisover2timeslargerthantheoneinthecaseofnoconsiderationofthepolaroneffects,andthetotalopticalabsorptionwillbebleachedatcenterwithinthephotonenergy.Thematrixelementenhancesitselfbecauseelectron-phononinteractionmakesthewavefunctionoftheelectionspreadtowiderspace,whichenhancestheoverlapofwavefunctions.

Fig.2Linear,third-ordernonlinearandtotalopticalabsorptioncurvesfortwocases:consideringelectron-LO-phononinteractioneffectsandignoreelectron-phononinteractioneffects.

InFig.3,thelinear,third-ordernonlinearandtotalopticalabsorptioncoefficientsareplottedasafunctionofthephotonenergy?ωwiththeincidentopticalintensityI=0.5×1010W/m2,R1=4.5 nm,R2=7.5 nm andd=4.0 nm for two cases: with electron-IO-phonon interaction effects and without electron-phonon interaction effects, which are illustrated by the dotted line and solid line, respectively. It can be shown that the electron-IO-phonon interaction effects on the optical absorption also make the linear absorption coefficient and the absolute value of third-order nonlinear absorption coefficient increase. Based on Fig.2 and Fig.3, we can also find that the influence of electron-LO-phonon interaction on the optical absorption is bigger than that of electron-IO-phonon interaction on the optical absorption. It shows that electron-LO-phonon interaction dominates the optical characters of electrons in low-dimensional system.

Fig.3 Linear, third-order nonlinear and total optical absorption curves for two cases: consider electron-IO-phonon interaction effects and ignore electron-phonon interaction effects.

In Fig.4, the total optical absorption coefficients are plotted as a function of the photon energy ?ωwithτ=300fs,R1=4.5 nm,R2=7.5 nm andd=4.0 nm for the different values of incident light intensities. It can been seen from Fig.4 that the total optical absorption coefficient will reduce significantly with the increasing of the incident optical intensityIwhen the polaron effects (solid line) are ignored. We also can see that the total optical absorption

Fig.4 Total optical absorption curves for different incident light intensities. Two cases, with and without LO phonon, and three intensities,I=0, 1.0, 2.0×1010W/m2arepresented.

willbestronglybleachedwhentheelectron-LO-phononinteraction(dottedline)isconsidered.WhentheincidentopticalintensityIexceeds the value ofI=2.0×1010W/m2,thepolaronabsorptionpeakwillbesignificantlysplitupintotwopeaks,whichisinconsequenceofthebleachingoftheabsorptionatlinearcenter.

InFig.5,thetotalopticalabsorptioncoefficientsareplottedasafunctionofthephotonenergy?ωwithτ=300fs,R1=4.5 nm,R2=7.5 nm andd=4.0 nm for two cases: electron-IO-phonon interaction effects and no electron-phonon interaction effects, which are illustrated by the dotted line and solid line, respectively. From Fig.5 we can see that the electron-IO-phonon interaction effects on the optical absorption also make the total optical absorption coefficient increase. From Fig.4 and Fig.5, we can also find that the influence of electron-LO-phonon interaction on the optical absorption is bigger than that of electron-IO-phonon interaction on the optical absorption.

Fig.5 Total optical absorption curves for different incident light intensities. Two cases, with and without IO phonon, and three intensities,I=0, 1.0, 2.0×1010W/m2arepresented.

InFig.6,thetotalopticalabsorptioncoefficientsareplottedasafunctionofthephotonenergy?ωwithI=0.5×1010W/m2,R1=4.5 nm,R2=7.5 nm andd=4.0 nm for three different values of the relaxation timeτ=50, 100, 200 fs. We can see that the total optical absorption coefficient will increase significantly with the relaxation timeτincreasingwhenweignorethepolaroneffects(solidline).Wealsocanseethatthetotalopticalabsorptionwillincreasestronglywhenweconsidertheelectron-LO-phononinteraction(dottedline).

Fig.6Totalopticalabsorptioncuresfordifferentrelaxationtimes.Twocases,withandwithoutLOphonon,andthreerelaxationtimes,τ=50, 100, 200 fs are presented.

In Fig.7, the total optical absorption coefficients are plotted as a function of the photon energy ?ωwithI=0.5×1010W/m2,R1=4.5 nm,R2=7.5 nm andd=4.0 nm for two cases: consider electron-IO-phonon interaction effects and ignore electron-phonon interaction effects, which are illustrated by the dotted line and solid line, respectively. From Fig.7, we can see that the electron-IO-phonon interaction effects on the optical absorption also make the total optical absorption coefficient increase. From

Fig.7 Total optical absorption cures for different relaxation times. Two cases, with and without IO phonon, and three relaxation times,τ=50, 100, 200 fs are presented.

Fig.6 and Fig.7, we can also find that the influence of IO phonon is smaller than that of LO phonon. In particular, the shift of total absorption peak is not distinct compared with that in Fig.6. Nevertheless, after considering the electron-IO-phonon interaction effect, the absorption peak is observed to become wider, which is remarkable like that in Fig.6. This verifies that polarization has a strong interaction with electromagnetic waves. Therefore, the polaron effect has a marked influence on the optical properties.

4 Conclusion

In this paper, we have researched the linear, third-order nonlinear, and total optical absorption coefficients of the weak-coupling optical polaron systems in the core-shell cylindrical quantum dots. The numerical calculations have been performed to study the total optical absorption coefficient of ZnS/CdSe core-shell cylindrical quantum dots by taking into account the influences of electron-LO-phonon and electron-IO-phonon interactions in this paper. The results show that the theoretical value of the optical absorption coefficient is greatly enhanced due to electron-phonon interaction effect. We also find that the influence of electron-LO-phonon interaction on the optical absorption is bigger than that of electron-IO-phonon interaction on the optical absorption. In addition, we find that the optical absorption coefficients are strongly affected by the incident optical intensity and the relaxation time. When the incident optical intensity becomes great enough the peaks of total optical absorption coefficients are split into two. Moreover, the correction of polaron effect to the energies of the electron makes the absorption peaks become wider. Therefore, the polaron effect has a marked influence on the optical properties.

[1] 于鳳梅, 郭康賢, 謝洪鯨, 等. Morse勢阱中子帶間的光吸收 [J]. 發光學報, 2003, 24(3):247-252. YU F M, GUO K X, XIE H J,etal.. Intersubband optical absorption in Morse quantum well [J].Chin.J.Lumin., 2003, 24(3):247-252. (in English)

[2] 申繼偉, 郭亨群, 呂蓬, 等. Si/SiNX超晶格材料的非線性光學特性 [J]. 發光學報, 2008, 29(6):1045-1049. SHEN J W, GUO X Q, LU P,etal.. Nonlinear optical properties of Si /SiNXsuperlattice [J].Chin.J.Lumin., 2008, 29(6):1045-1049. (in Chinese)

[3] 陳知紅, 方天紅, 李錢光, 等. 極化子效應對ZnS/CdSe柱型核殼量子點簡并四波混頻過程的影響 [J]. 光子學報, 2015, 44(4):0419003. CHEN Z H, FANG T H, LI Q G,etal.. Polaron effect on the degenerate four-wave mixing in a ZnS/CdSe quantum dot quantum well [J].ActaPhoton.Sinica, 2015, 44(4):0419003. (in Chinese).

[4] BOUZAIENE L, ALAMRI H, SFAXI L,etal.. Simultaneous effects of hydrostatic pressure, temperature and electric field on optical absorption in InAs/GaAs lens shape quantum dot [J].J.AlloysCompd., 2016, 655:172-177.

[5] LIU K, SCHMEDAKE T A, DANESHVAR K,etal.. Interaction of CdSe/ZnS quantum dots: among themselves and with matrices [J].Microelectron.J., 2007, 38(6):700-705.

[6] FENG X, XIONG G, ZHANG X,etal.. Third-order nonlinear optical susceptibilities associated with intersubband transitions in CdSe/ZnS core-shell quantum dots [J].PhysicaB:CondensedMatter, 2006, 383(2):207-212.

[7] 陳知紅, 王軍延, 方天紅. 極化子效應對ZnS/CdSe量子點三階極化率的影響 [J]. 發光學報, 2009, 30(4):535-540. CHEN Z H, WANG J Y, FANG T H. Effect of polaron effect on third-order susceptibility in ZnS/CdSe quantum dot quantum well [J].Chin.J.Lumin., 2009, 30(4):535-540. (in Chinese).

[8] NAIMI Y, JAFARI A R. Oscillator strengths of the intersubband electronic transitions in the multi-layered nano-antidots with hydrogenic impurity [J].J.Comput.Electron., 2012, 11(4):414-420.

[9] XIE W L. Absorption spectra and refractive index changes of an exciton in a core/shell quantum dot [J].Commun.Theor.Phys., 2015, 63(5):635.

[10] ZHANG C J, GUO K X. Polaron effects on the optical absorptions in asymmetrical semi-parabolic quantum wells [J].PhysicaE, 2007, 39(1):103-108.

[11] YAKAR Y, ?AKIR B, ?ZMEN A. Calculation of linear and nonlinear optical absorption coefficients of a spherical quantum dot with parabolic potential [J].Opt.Commun., 2010, 283(9):1795-1800.

[12] YESILGUL U, UNGAN F, SAKIROGLU S,etal.. Effect of intense high-frequency laser field on the linear and nonlinear intersubband optical absorption coefficients and refractive index changes in a parabolic quantum well under the applied electric field [J].J.Lumin., 2014, 145:379-386.

[13] 于鳳梅, 王克強, 申朝文. 極化子效應對非對稱量子阱中光吸收系數的影響 [J]. 發光學報, 2010, 31(4):467-472. YU F M, WANG K Q, SHEN C W. Influence of polaron effects on the optical absorptions in asymmetrical quantum wells [J].Chin.J.Lumin., 2010, 31(4):467-472. (in English)

[14] GAMBHIR M, KUMAR M, JHA P K,etal.. Linear and nonlinear optical absorption coefficients and refractive index changes associated with intersubband transitions in a quantum disk with flat cylindrical geometry [J].J.Lumin., 2013, 143:361-367.

[15] GUO K X, XIAO B, ZHOU Y,etal.. Polaron effects on the third-harmonic generation in asymmetrical semi-exponential quantum wells [J].J.Opt., 2015, 17(3):035505.

[16] MOU S, GUO K, XIAO B. Polaron effects on the linear and nonlinear intersubband optical absorption coefficients in quantum wells with asymmetrical semi-exponential potential [J].Superlatt.Microstruct., 2014, 72:72-82.

[17] CHEN Z, YAO D, ZHANG X,etal.. Polaron effect-dependent third-order optical susceptibility in a ZnS/CdSe quantum dot quantum well [J].Microelectron.J., 2008, 39(12):1654-1658.

[18] XIE H J, CHEN C Y, MA B K. The bound polaron in a cylindrical quantum well wire with a finite confining potential [J].J.Phys.:CondensedMatter, 2000, 12(40):8623-8640.

[19] ZHANG X, XIONG G, FENG X. Well width-dependent third-order optical nonlinearities of a ZnS/CdSe cylindrical quantum dot quantum well [J].PhysicaE, 2006, 33(1):120-124.

[20] ALCALDE A M, MARQUES G E. Electron-optical-phonon scattering rates in spherical CdSe quantum dots in an external magnetic field [J].Phys.Rev. B, 2002, 65(11):113301.

陳知紅(1980-)，女，湖北公安人，碩士，副教授，2007年于武漢大學獲得碩士學位，主要從事非線性光學方面的研究。

E-mail: zhihong9905@163.com李錢光(1978-)，男，湖北廣水人，博士，副教授，2010年于華中科技大學獲得博士學位，主要從事飛秒激光脈沖與原子、分子相互作用的理論研究。

E-mail: liqianguang@126.com

2016-12-13；

2017-02-03

國家自然科學基金(11547018)； 湖北省教育廳研究項目(Q20142706)； 湖北工程學院自然科學基金(z2013028)； 湖北省自然科學基金(2014CFB579)資助項目 Supported by National Natural Science Foundation of China(11547018); Research Foundation of Education Bureau of Hubei Province(Q20142706); Natural Science Foundation of Hubei Engineering University(z2013028); Natural Science Foundation of Hubei Province(2014CFB579)

極化子效應對ZnS/CdSe核殼量子點光吸收系數的影響

陳知紅， 李錢光*， 易煦農， 余華清， 熊良斌

(湖北工程學院 物理與電子信息工程學院， 湖北 孝感 432000)

在有效質量近似下，利用量子力學密度矩陣理論，從理論上研究了考慮極化子效應后核殼量子點中線性、三階非線性以及總的光吸收系數在不同條件下隨入射光能量變化的關系。通過數值計算，分析了電子-LO聲子和電子-IO聲子相互作用對ZnS/CdSe柱型核殼結構量子點光吸收系數的影響。結果表明，極化子效應對光吸收系數有很大影響，不同聲子模式對光吸收系數影響大小不同。考慮電子-LO聲子后，光吸收系數被大大提高。另外，入射光強和弛豫時間對系統的吸收系數也有很大影響。

極化子； 核-殼量子點； 光吸收

1000-7032(2017)05-0580-07

O437; O472.3 Document code： A

10.3788/fgxb20173805.0580

*CorrespondingAuthor,E-mail:liqianguang@126.com