Colloidal semiconductor quantum dots (QDs) are promising building blocks for the realization of future optoelectronic technologies, thanks to their size-tunable electronic and optical properties. Among various types of QDs, colloidal "giant" QDs (g-QDs, core/thick-shell) have been widely used in different applications, such as solar cells, light emitting devices, luminescent solar concentrators and photoelectrochemical (PEC) hydrogen production. However, g-QDs have a thick-shell which serves as a physical barrier for electron and hole transfer, leading to a slow charge transfer rate. In this work, we synthesized CdSe/CdSexS1-x/CdS core/shell/shell g-QDs with an intermediate CdSexS1-x alloyed layer. The presence of this interfacial layer largely improves the absorption of CdSe/CdS QDs, particularly in the 300-650 nm range. By engineering the interfacial layer, the holes can leak more into the CdS shell region compared to that of CdSe/CdS QDs. PEC devices based on alloyed g-QDs exhibit a 20% higher saturated photocurrent density (11 ± 0.5 mA cm-2) compared to CdSe/CdS QDs. In addition, after one-hour illumination (100 mW cm-2), the PEC cell based on alloyed g-QDs still exhibits a photocurrent density of 7.5 mA cm-2, maintaining 70% of its initial value. Such alloyed g-QDs are very promising for several emerging optoelectronic applications, where charge separation, transfer and transport play a critical role for the realization of high performance devices.
Colloidal semiconductor quantum dots (QDs) are promising building blocks for the realization of future optoelectronic technologies, thanks to their size-tunable electronic and optical properties. Among various types of QDs, colloidal "giant" QDs (g-QDs, core/thick-shell) have been widely used in different applications, such as solar cells, light emitting devices, luminescent solar concentrators and photoelectrochemical (PEC) hydrogen production. However, g-QDs have a thick-shell which serves as a physical barrier for electron and hole transfer, leading to a slow charge transfer rate. In this work, we synthesized CdSe/CdSexS1-x/CdS core/shell/shell g-QDs with an intermediate CdSexS1-x alloyed layer. The presence of this interfacial layer largely improves the absorption of CdSe/CdS QDs, particularly in the 300-650 nm range. By engineering the interfacial layer, the holes can leak more into the CdS shell region compared to that of CdSe/CdS QDs. PEC devices based on alloyed g-QDs exhibit a 20% higher saturated photocurrent density (11 +/- 0.5 mA cm(-2)) compared to CdSe/CdS QDs. In addition, after one-hour illumination (100 mW cm(-2)), the PEC cell based on alloyed g-QDs still exhibits a photocurrent density of 7.5 mA cm(-2), maintaining 70% of its initial value. Such alloyed g-QDs are very promising for several emerging optoelectronic applications, where charge separation, transfer and transport play a critical role for the realization of high performance devices.
Tailoring the interfacial structure of colloidal "giant" quantum dots for optoelectronic applications
Vomiero, Alberto
;
2018-01-01
Abstract
Colloidal semiconductor quantum dots (QDs) are promising building blocks for the realization of future optoelectronic technologies, thanks to their size-tunable electronic and optical properties. Among various types of QDs, colloidal "giant" QDs (g-QDs, core/thick-shell) have been widely used in different applications, such as solar cells, light emitting devices, luminescent solar concentrators and photoelectrochemical (PEC) hydrogen production. However, g-QDs have a thick-shell which serves as a physical barrier for electron and hole transfer, leading to a slow charge transfer rate. In this work, we synthesized CdSe/CdSexS1-x/CdS core/shell/shell g-QDs with an intermediate CdSexS1-x alloyed layer. The presence of this interfacial layer largely improves the absorption of CdSe/CdS QDs, particularly in the 300-650 nm range. By engineering the interfacial layer, the holes can leak more into the CdS shell region compared to that of CdSe/CdS QDs. PEC devices based on alloyed g-QDs exhibit a 20% higher saturated photocurrent density (11 +/- 0.5 mA cm(-2)) compared to CdSe/CdS QDs. In addition, after one-hour illumination (100 mW cm(-2)), the PEC cell based on alloyed g-QDs still exhibits a photocurrent density of 7.5 mA cm(-2), maintaining 70% of its initial value. Such alloyed g-QDs are very promising for several emerging optoelectronic applications, where charge separation, transfer and transport play a critical role for the realization of high performance devices.
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