One Pot Synthesis of Cyan Emitting CdZnSSe Quantum Dots for Human Centric Lighting

IF 3.3 3区 化学 Q2 CHEMISTRY, PHYSICAL
Abraham J. Jordan, Zhuolei Zhang, Ellie Bennett, Leslie Guadalupe Castro, David Jingbo Han, Iva Rreza, Ayelet Teitelboim, Brian Theobald, Bereket Zekarias, Emory M. Chan, Jonathan S. Owen
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Abstract

A one pot synthesis of blue and green emissive CdZnSSe quantum dots (QDs) from thio- and selenoureas and Cd and Zn carboxylates is optimized using high throughput robotic optimization. A large set of spectral data (N = 192) is used to train machine learning models that accurately predict the photoluminescence emission wavelength (λmax) and full-width half-maximum, and the relative photoluminescence quantum yield (PLQY) from the S:Se and Zn:Cd stoichiometries and reaction time. ZnS shells are deposited on the crude QD heterostructures using 4-tert-butylbenzyl mercaptan, a more reactive source of sulfide that enables shell growth below the temperature where ion diffusion in the QD can broaden its optical spectrum (≤275 °C). These optimized procedures provide gram quantities of blue-green emitting QDs (PLQY = 85–99%) in a single reaction vessel. A solid state lighting device (4260 K) that incorporates cyan emissive QDs achieved a higher luminous efficacy of 179 lm/W and melanopic daylight efficiency ratio (0.71) than existing commercial human centric lighting devices.

Abstract Image

一锅合成用于以人为本照明的青色发光 CdZnSSe 量子点
利用高通量机器人优化技术,从硫代和硒代脲类以及镉和锌羧酸盐中一锅合成蓝绿发射型 CdZnSSe 量子点 (QDs)。大量光谱数据(N = 192)被用于训练机器学习模型,该模型可根据 S:Se 和 Zn:Cd 的化学计量学和反应时间准确预测光致发光发射波长 (λmax) 和全宽半最大值,以及相对光致发光量子产率 (PLQY)。ZnS 外壳是用 4-叔丁基苄基硫醇沉积在粗制 QD 异质结构上的,硫醇是一种活性更强的硫化物,它能使外壳在 QD 中离子扩散能扩大其光学光谱的温度(≤275 ℃)以下生长。这些优化程序可在单个反应容器中提供克级数量的蓝绿发光 QDs(PLQY = 85-99%)。与现有的以人为中心的商业照明设备相比,采用青色发光 QDs 的固态照明设备(4260 K)的光效高达 179 lm/W,黑色素日光效率比为 0.71。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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