CdSe_xS_（1-x）和CdSe_xS_（1-x）/ZnS系列量子点的光谱与光学非线性特性研究
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摘要
半导体量子点具有大的非线性吸收系数和非线性折射率,使之成为光开关、光限幅和光存储等光电子器件的优选材料。因此研究量子点的非线性光学特性,探索其产生各种光学特性的机理以及其潜在的应用具有非常重要的意义。本文以不同组分的非核壳CdSe_xS_(1-x),和核壳CdSe_xS_(1-x)/ZnS系列量子点为研究对象,围绕不同组分、包壳与未包壳量子点的光谱特性,非线性光学特性以及光限幅效应等方面进行了系统的研究。主要工作归纳如下:
1.研究了不同组分的CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点的吸收光谱特征和荧光光谱特性。首先,通过吸收光谱与有效质量近似模型,确定了CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点的组分,比按投料计量的组分准确的多,并发现组分能够调谐吸收光谱波长与发射波长。其次,通过对吸收光谱进行高斯拟合,计算了CdSe_xS_(1-x)和CdSe_(1-x)S_x/ZnS系列量子点的本征复合寿命,发现通过壳层对量子点的修饰,能够缩短本征复合寿命,增加了振子强度;通过比较CdSe_(1-x)S_x和CdSe_(1-x)S_x/ZnS系列量子点荧光光谱,发现核壳结构的量子点荧光光谱强度明显增强;这表明包覆壳层对量子点修饰能够减少量子点表面缺陷密度,减小了无辐射跃迁的通道,从而能够提高量子点的荧光强度。
2.在波长为1064nm皮秒激光激发下,用Z-扫描方法研究了不同组分的CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点非线性光学特性。结果表明CdSe_(0.5)S_(0.5)/ZnS量子点对1064nm的激发光存在非线性吸收,CdSe_(0.3)S_(0.7)、CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.8)S_(0.2)/ZnS和CdSe_(0.3)S_(0.7)/ZnS量子点没有非线性吸收。首先建立双光子激发的动力学能级模型,解释了CdSe_(0.5)S_(0.5)/ZnS量子点的非线性折射率随入射光强的增加线性减小的变化规律,求得该量子点溶液的三阶非线性折射率γ_3=1.50×10~(-17)m~2/W(SI)(5.1×10~(-11)esu),自由载流子折射截面为σ_r=-6.74×10~(-24)cm~3,双光子吸收截面δ_(2 PA)达到10~4GM数量级。其次,通过闭孔Z-扫描技术求得CdSe_(0.3)S_(0.7)、CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.8)S_(0.2)/ZnS和CdSe_(0.3)S_(0.7)/ZnS量子点不同入射光强的非线性折射率,发现其非线性折射率随入射光强的变化不大,这是因为1064nm的激发光不在量子点的吸收区内,所以其非线性折射率主要来源于价带的束缚电子,激发光只引起价带束缚电子的电子云畸变,对束缚电子的分布影响不大。还发现随着Se的增加,CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点的非线性折射率随之增大,并对此给出了定性的解释。这说明组分不仅可以调谐量子点的发射波长,还可以调谐量子点的非线性折射率。另外,包覆壳层量子点的非线性折射率比相同组分的非核壳量子点大,说明壳层包覆能够改善其光学非线性特性。
3.在波长为532nm的皮秒激光激发下,用Z-扫描方法研究了不同组分的CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点非线性光学特性。结果表明这些量子点对532nm的激发光都存在非线性吸收,其中CdSe_(0.3)S_(0.7)量子点的非线性吸收源于双光子吸收和双光子诱导的激发态吸收过程,其余量子点的非线性吸收皆源于激发态吸收过程。首先建立双光子激发动力学能级模型解释了CdSe_(0.3)S_(0.7)量子点有效的双光子吸收系数随入射光强增大线性增大和非线性折射率随入射光强增大线性减小的现象,这表明其非线性折射率主要源于价带束缚电子和双光子产生的自由载流子的共同贡献,且双光子诱导的激发态吸收和自由载流子的非线性响应都是五阶非线性过程。求得双光子吸收系数1.2cm/GW,双光子吸收截面δ_(2PA)=1.5×10~4GM,双光子吸收诱导的激发态吸收截面δ_(eff)=0.63×10~(-19)cm~2,三阶非线性折射率为2.6×10~(-14)cm~2/W(8.7×10~(-12)esu),其自由载流子的折射截面σ_r,=-2.9×10~(-23)cm~3。其次,建立激发态吸收的动力学能级模型解释了CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.3)S_(0.7)/ZnS、CdSe_(0.5)S_(0.5)/ZnS和CdSe_(0.8)S_(0.2)/ZnS量子点在单光子共振区的非线性吸收现象,证实其源于激发态吸收,并求得了这些量子点的有效的激发态吸收截面和非线性折射率,发现随着Se的增加,非线性折射率增加,而有效的激发态吸收截面减小,说明组分能够调谐量子点的光学非线性特性,并定性地解释了这种变化规律;另外,还发现包覆壳层的量子点的有效激发态吸收截面和非线性折射率都比同组分的未包壳量子点大,说明表面包覆能够有效地改善量子点的非线性光学特性。
4.通过测量量子点的非线性透过率,发现随入射光强的增加,非线性透过率很快减小,表明这些量子点具有良好的光限幅行为,可以作为光限幅器的优选材料。
The quantum dots(QDs) possess the large nonlinear absorption coefficient and nonlinear refractive index, which enable them to be the candidates for the all-optical switching and optical limiter. Therefore, it is very significant that their optical nonlinearity, their physical mechanism and their potential application are investigated. In this dissertation, we chose a series of CdSe_xS_(1-x)and CdSe_xS_(1-x)/ZnS QDs as the research object, and discus the effects of the composition and shell of QDs on the spectra. Their nonlinear optical properties have been investigated by Z-scan technique. At last, the potential application in optical limiting also has been attempted for these QDs. The main results of the research work are as follows:
1.A detailed analysis of the series of CdSe_xS_(1-x)and CdSe_xS_(1-x)/ZnS QDs was presented by means of absorption and fluorescence spectra. First, based on the absorption spectra and effective mass approximation, the composition of these QDs was determined, which is more accurate than feed ratio; it was also found that the spectra properties can be tuned by the composition. Second, the intrinsic radiative lifetime of these QDs was determined on the basis of the Gaussian fitting for the absorption spectra; it was found that the intrinsic radiative lifetime is decreased and the oscillator strength is enhanced by the surface modification of shell structure. Comparing the fluorescence spectra of core-shell QDs with that of their counterpart, it was found that the fluorescence intensity is enhanced by surface modification. These results indicate that surface modification can reduce their defect concentration, which results in the decrease of non-radiative channel and enhancement of fluorescent intensity.
2.We investigated the optical nonlinearity of the different composition of the non-core/shell and core/shell QDs with 1064nm ps pulse by Z-scan technique. The Z-scan results show that two-photon absorption(TPA) occurred for core/shell CdSe_(0.5)S_(0.5)/ZnS QDs, and no TPA occurred for the others, including CdSe_(0.3)S_(0.7)、CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.8)S_(0.2)、/ZnS and CdSe_(0.3)S_(0.7)/ZnS QDs. First, we established the energy level model of the optical physical process and interpreted the change of the nonlinear refractive indices with the increase of input intensity; the third-order nonlinear indices is determined to be 1.50×10~(-17)m~2/W(SI)(5.1×10~(-11)esu), the refraction cross section is 6.74×10~(-24)cm~3, their average TPA cross section is up to the order of 1.3×10~4GM. Second, the nonlinear refractive indices of CdSe_(0.3)S_(0.7)、CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.8)S_(0.2)/ZnS and CdSe_(0.3)S_(0.7)/ZnS QDs is obtained by close-aperture Z-scan, it was found that their nonlinear refractive indices hardly vary with input intensity. Base on the experimental results, the optical nonlinearity in the nonresonant region is ascribed to the bound electronic response, which results from the distortion of electron clound and indicate that the input intensity have less influence on them. It was also found that the nonlinear refractive indices increase with the decrease of bandgap, which is caused by Se content in these QDs. Then we give a qualitative explanation for this phenomenon. This result shows that not only the peak wavelength of these QDs but their nonlinear optical properties can be altered by composition of these QDs. Moreover, the nonlinear refractive indices of core/shell QDs is larger than the counterpart with the same composition, which indicates that surface modification by coating shell structure on the QDs can improve their nonlinear optical properties.
3. We investigated the optical nonlinearity of a series of CdSe_xS_(1-x) and CdSe_xS_(1-x)/ZnS QDs with 532nm ps pulse by Z-scan technique. The Z-scan results show that the nonlinear absorption occurred for all the QDs. Among them, the nonlinear absorption of CdSe_(0.3)S_(0.7) QDs originates from TPA process and the TPA-induced excited state absorption(TPESA) process, that of the other QDs originates from excited state absorption(ESA). First, based on the energy leve model of two-photon-excitation dynamics, we interpreted the phenomena that their TPA coefficients linearly increase with increase of input intensity and their nonlinear refractive indices linearly decrease with input intensity. This result shows that the nonlinear refractive index is ascribed to the contribution of bond electronics and TPA-generated free carriers. Both the TPESA and the nonlinear response of TPA-generated free carriers are fifth-order nonlinear process. The TPA coefficient of CdSe_(0.3)S_(0.7) QDs is 1.2cm/GW by open-aperture Z-scan, their TPA cross section is 1.5×10~4GM, the TPA-induced ESA cross section is 0.63×10~(-19)cm~2, the third-order nonlinear index is 2.6×10~(-14)cm~2/W(8.7×10~(-12)esu) and the refraction cross section of free carrier is -2.9×10~(-23)cm~3. Second, in order to interpret the nonlinear absorption of CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.3)S_(0.7)/ZnS、CdSe_(0.5)S_(0.5)/ZnS and CdSe_(0.8)S_(0.2)/ZnS QDs in resonant region, the energy level model of ESA dynamics is established. It is confirmed that the nonlinear absorption originates from ESA. The ESA cross sections and the nonlinear refractive of these QDs are determined by Z-scan. It was found that the nonlinear refractive indices for these QDs increase with the increase of Se content while their ESA cross sections decrease with it, for which a qualitative explanation is presented by us. Moreover, we also found that the QDs with ZnS shell exhibit larger ESA cross section and nonlinear refractive indices than their counterpart, which confirms that surface modification can improve the nonlinear optical properties.
4. Through the measure of nonlinear transmittance of these QDs, it was found that the nonlinear transmittance decreases fast with input intensty. The result shows that these QDs exhibit excellent optical limiting properties, which enable them to be a promising candidate material for optical limiters.
1.研究了不同组分的CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点的吸收光谱特征和荧光光谱特性。首先,通过吸收光谱与有效质量近似模型,确定了CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点的组分,比按投料计量的组分准确的多,并发现组分能够调谐吸收光谱波长与发射波长。其次,通过对吸收光谱进行高斯拟合,计算了CdSe_xS_(1-x)和CdSe_(1-x)S_x/ZnS系列量子点的本征复合寿命,发现通过壳层对量子点的修饰,能够缩短本征复合寿命,增加了振子强度;通过比较CdSe_(1-x)S_x和CdSe_(1-x)S_x/ZnS系列量子点荧光光谱,发现核壳结构的量子点荧光光谱强度明显增强;这表明包覆壳层对量子点修饰能够减少量子点表面缺陷密度,减小了无辐射跃迁的通道,从而能够提高量子点的荧光强度。
2.在波长为1064nm皮秒激光激发下,用Z-扫描方法研究了不同组分的CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点非线性光学特性。结果表明CdSe_(0.5)S_(0.5)/ZnS量子点对1064nm的激发光存在非线性吸收,CdSe_(0.3)S_(0.7)、CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.8)S_(0.2)/ZnS和CdSe_(0.3)S_(0.7)/ZnS量子点没有非线性吸收。首先建立双光子激发的动力学能级模型,解释了CdSe_(0.5)S_(0.5)/ZnS量子点的非线性折射率随入射光强的增加线性减小的变化规律,求得该量子点溶液的三阶非线性折射率γ_3=1.50×10~(-17)m~2/W(SI)(5.1×10~(-11)esu),自由载流子折射截面为σ_r=-6.74×10~(-24)cm~3,双光子吸收截面δ_(2 PA)达到10~4GM数量级。其次,通过闭孔Z-扫描技术求得CdSe_(0.3)S_(0.7)、CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.8)S_(0.2)/ZnS和CdSe_(0.3)S_(0.7)/ZnS量子点不同入射光强的非线性折射率,发现其非线性折射率随入射光强的变化不大,这是因为1064nm的激发光不在量子点的吸收区内,所以其非线性折射率主要来源于价带的束缚电子,激发光只引起价带束缚电子的电子云畸变,对束缚电子的分布影响不大。还发现随着Se的增加,CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点的非线性折射率随之增大,并对此给出了定性的解释。这说明组分不仅可以调谐量子点的发射波长,还可以调谐量子点的非线性折射率。另外,包覆壳层量子点的非线性折射率比相同组分的非核壳量子点大,说明壳层包覆能够改善其光学非线性特性。
3.在波长为532nm的皮秒激光激发下,用Z-扫描方法研究了不同组分的CdSe_xS_(1-x)和CdSe_xS_(1-x)/ZnS系列量子点非线性光学特性。结果表明这些量子点对532nm的激发光都存在非线性吸收,其中CdSe_(0.3)S_(0.7)量子点的非线性吸收源于双光子吸收和双光子诱导的激发态吸收过程,其余量子点的非线性吸收皆源于激发态吸收过程。首先建立双光子激发动力学能级模型解释了CdSe_(0.3)S_(0.7)量子点有效的双光子吸收系数随入射光强增大线性增大和非线性折射率随入射光强增大线性减小的现象,这表明其非线性折射率主要源于价带束缚电子和双光子产生的自由载流子的共同贡献,且双光子诱导的激发态吸收和自由载流子的非线性响应都是五阶非线性过程。求得双光子吸收系数1.2cm/GW,双光子吸收截面δ_(2PA)=1.5×10~4GM,双光子吸收诱导的激发态吸收截面δ_(eff)=0.63×10~(-19)cm~2,三阶非线性折射率为2.6×10~(-14)cm~2/W(8.7×10~(-12)esu),其自由载流子的折射截面σ_r,=-2.9×10~(-23)cm~3。其次,建立激发态吸收的动力学能级模型解释了CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.3)S_(0.7)/ZnS、CdSe_(0.5)S_(0.5)/ZnS和CdSe_(0.8)S_(0.2)/ZnS量子点在单光子共振区的非线性吸收现象,证实其源于激发态吸收,并求得了这些量子点的有效的激发态吸收截面和非线性折射率,发现随着Se的增加,非线性折射率增加,而有效的激发态吸收截面减小,说明组分能够调谐量子点的光学非线性特性,并定性地解释了这种变化规律;另外,还发现包覆壳层的量子点的有效激发态吸收截面和非线性折射率都比同组分的未包壳量子点大,说明表面包覆能够有效地改善量子点的非线性光学特性。
4.通过测量量子点的非线性透过率,发现随入射光强的增加,非线性透过率很快减小,表明这些量子点具有良好的光限幅行为,可以作为光限幅器的优选材料。
The quantum dots(QDs) possess the large nonlinear absorption coefficient and nonlinear refractive index, which enable them to be the candidates for the all-optical switching and optical limiter. Therefore, it is very significant that their optical nonlinearity, their physical mechanism and their potential application are investigated. In this dissertation, we chose a series of CdSe_xS_(1-x)and CdSe_xS_(1-x)/ZnS QDs as the research object, and discus the effects of the composition and shell of QDs on the spectra. Their nonlinear optical properties have been investigated by Z-scan technique. At last, the potential application in optical limiting also has been attempted for these QDs. The main results of the research work are as follows:
1.A detailed analysis of the series of CdSe_xS_(1-x)and CdSe_xS_(1-x)/ZnS QDs was presented by means of absorption and fluorescence spectra. First, based on the absorption spectra and effective mass approximation, the composition of these QDs was determined, which is more accurate than feed ratio; it was also found that the spectra properties can be tuned by the composition. Second, the intrinsic radiative lifetime of these QDs was determined on the basis of the Gaussian fitting for the absorption spectra; it was found that the intrinsic radiative lifetime is decreased and the oscillator strength is enhanced by the surface modification of shell structure. Comparing the fluorescence spectra of core-shell QDs with that of their counterpart, it was found that the fluorescence intensity is enhanced by surface modification. These results indicate that surface modification can reduce their defect concentration, which results in the decrease of non-radiative channel and enhancement of fluorescent intensity.
2.We investigated the optical nonlinearity of the different composition of the non-core/shell and core/shell QDs with 1064nm ps pulse by Z-scan technique. The Z-scan results show that two-photon absorption(TPA) occurred for core/shell CdSe_(0.5)S_(0.5)/ZnS QDs, and no TPA occurred for the others, including CdSe_(0.3)S_(0.7)、CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.8)S_(0.2)、/ZnS and CdSe_(0.3)S_(0.7)/ZnS QDs. First, we established the energy level model of the optical physical process and interpreted the change of the nonlinear refractive indices with the increase of input intensity; the third-order nonlinear indices is determined to be 1.50×10~(-17)m~2/W(SI)(5.1×10~(-11)esu), the refraction cross section is 6.74×10~(-24)cm~3, their average TPA cross section is up to the order of 1.3×10~4GM. Second, the nonlinear refractive indices of CdSe_(0.3)S_(0.7)、CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.8)S_(0.2)/ZnS and CdSe_(0.3)S_(0.7)/ZnS QDs is obtained by close-aperture Z-scan, it was found that their nonlinear refractive indices hardly vary with input intensity. Base on the experimental results, the optical nonlinearity in the nonresonant region is ascribed to the bound electronic response, which results from the distortion of electron clound and indicate that the input intensity have less influence on them. It was also found that the nonlinear refractive indices increase with the decrease of bandgap, which is caused by Se content in these QDs. Then we give a qualitative explanation for this phenomenon. This result shows that not only the peak wavelength of these QDs but their nonlinear optical properties can be altered by composition of these QDs. Moreover, the nonlinear refractive indices of core/shell QDs is larger than the counterpart with the same composition, which indicates that surface modification by coating shell structure on the QDs can improve their nonlinear optical properties.
3. We investigated the optical nonlinearity of a series of CdSe_xS_(1-x) and CdSe_xS_(1-x)/ZnS QDs with 532nm ps pulse by Z-scan technique. The Z-scan results show that the nonlinear absorption occurred for all the QDs. Among them, the nonlinear absorption of CdSe_(0.3)S_(0.7) QDs originates from TPA process and the TPA-induced excited state absorption(TPESA) process, that of the other QDs originates from excited state absorption(ESA). First, based on the energy leve model of two-photon-excitation dynamics, we interpreted the phenomena that their TPA coefficients linearly increase with increase of input intensity and their nonlinear refractive indices linearly decrease with input intensity. This result shows that the nonlinear refractive index is ascribed to the contribution of bond electronics and TPA-generated free carriers. Both the TPESA and the nonlinear response of TPA-generated free carriers are fifth-order nonlinear process. The TPA coefficient of CdSe_(0.3)S_(0.7) QDs is 1.2cm/GW by open-aperture Z-scan, their TPA cross section is 1.5×10~4GM, the TPA-induced ESA cross section is 0.63×10~(-19)cm~2, the third-order nonlinear index is 2.6×10~(-14)cm~2/W(8.7×10~(-12)esu) and the refraction cross section of free carrier is -2.9×10~(-23)cm~3. Second, in order to interpret the nonlinear absorption of CdSe_(0.5)S_(0.5)、CdSe_(0.8)S_(0.2)、CdSe_(0.3)S_(0.7)/ZnS、CdSe_(0.5)S_(0.5)/ZnS and CdSe_(0.8)S_(0.2)/ZnS QDs in resonant region, the energy level model of ESA dynamics is established. It is confirmed that the nonlinear absorption originates from ESA. The ESA cross sections and the nonlinear refractive of these QDs are determined by Z-scan. It was found that the nonlinear refractive indices for these QDs increase with the increase of Se content while their ESA cross sections decrease with it, for which a qualitative explanation is presented by us. Moreover, we also found that the QDs with ZnS shell exhibit larger ESA cross section and nonlinear refractive indices than their counterpart, which confirms that surface modification can improve the nonlinear optical properties.
4. Through the measure of nonlinear transmittance of these QDs, it was found that the nonlinear transmittance decreases fast with input intensty. The result shows that these QDs exhibit excellent optical limiting properties, which enable them to be a promising candidate material for optical limiters.
引文
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