Murray Ian M, Choi Sinil, Jemison Henry M, Kim Sunghu, Altman Alison B, Jeong Sohee, Son Dong Hee
Department of Chemistry, Texas A&M University, College Station, Texas 77843, USA.
Department of Energy Science, Sungkyunkwan University, Seobu-ro, Jangan-gu, Suwon-si, Gyeonggi-do, Republic of Korea.
J Chem Phys. 2025 Jul 14;163(2). doi: 10.1063/5.0270400.
We investigated the pressure-dependent exciton absorption and photoluminescence (PL) properties of colloidal InAs/ZnSe core/shell quantum dots (QDs) emitting near-infrared (NIR) photons, an environmentally friendly alternative to heavy-metal-containing NIR QDs. A detailed analysis of exciton absorption and emission spectra was conducted in the pressure range of 0-10 GPa, focusing on the energy shifts, PL intensity, and lineshape changes with pressure. The pressure coefficients for exciton absorption and PL peaks were ∼70% of the bulk InAs value, with enhanced bandgap nonlinearity tentatively attributed to the higher bulk modulus of QDs compared to bulk material. The pressure-induced shifts in exciton absorption and PL peaks were reversible upon compression and decompression, with no indication of the semiconductor-to-metallic phase transition observed in bulk InAs around 7 GPa. However, PL intensity exhibited partial irreversibility, suggesting defect formation at the core/shell interface under pressure. From the findings of this study, along with previous high-pressure studies on molecular beam epitaxy-grown InAs QDs on GaAs, we infer the importance of the shell in determining the pressure response of exciton absorption and PL in core/shell QD structures with non-negligible interfacial strain and wave function spill into the shell.
我们研究了发射近红外(NIR)光子的胶体InAs/ZnSe核壳量子点(QD)的压力依赖激子吸收和光致发光(PL)特性,它是含重金属近红外量子点的一种环境友好替代品。在0至10吉帕的压力范围内,对激子吸收和发射光谱进行了详细分析,重点关注能量位移、PL强度以及随压力的线形变化。激子吸收和PL峰的压力系数约为体相InAs值的70%,带隙非线性增强初步归因于量子点与体相材料相比具有更高的体模量。激子吸收和PL峰的压力诱导位移在压缩和减压时是可逆的,未观察到在约7吉帕时体相InAs中出现的半导体到金属的相变迹象。然而,PL强度表现出部分不可逆性,表明在压力下核壳界面处形成了缺陷。根据本研究的结果,以及之前对在GaAs上分子束外延生长的InAs量子点的高压研究,我们推断壳层在确定具有不可忽略的界面应变和波函数泄漏到壳层的核壳量子点结构中激子吸收和PL的压力响应方面的重要性。