Semiconductor quantum dots (QDs) hold great potential for solid-state light-emitting devices and optical and spin-based quantum information processing, but the efficiency of QD-based spin LEDs remains limited, and their physics not fully understood. Using tunable laser spectroscopy, the authors discover that here an intrinsic obstacle to spin generation is $p\phantom{\rule{0}{0ex}}h\phantom{\rule{0}{0ex}}o\phantom{\rule{0}{0ex}}n\phantom{\rule{0}{0ex}}o\phantom{\rule{0}{0ex}}n$ $b\phantom{\rule{0}{0ex}}o\phantom{\rule{0}{0ex}}t\phantom{\rule{0}{0ex}}t\phantom{\rule{0}{0ex}}l\phantom{\rule{0}{0ex}}e\phantom{\rule{0}{0ex}}n\phantom{\rule{0}{0ex}}e\phantom{\rule{0}{0ex}}c\phantom{\rule{0}{0ex}}k$, a lack of phonon-mediated relaxation pathways that can arise in a zero-dimensional system. This insight provides design rules for energy-level engineering in spin-optoelectronic applications of QDs, yielding about a threefold increase in spin generation efficiency, even at elevated temperatures.
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