Spatial and Intensity Modulation of Nanowire Emission Induced by Mobile Charges

摘要

Single-molecule optical experiments carried out in conjunction with externally applied electric fields show deliberate spatial and intensity control over CdSe nanowire (NW) emission. In particular, by applying external fields to electrically isolated (single) NWs, their emission can be localized in areas of the wire closest to the positive electrode. In a few cases, the resulting emission intensity increases over the corresponding zero-field value by nearly an order of magnitude. More often than not, factors of 2-3 are seen. Reversing the field polarity causes the emission to localize in opposite regions of the wire. Emission from individual NWs can therefore be modulated. Complementary ac electric field measurements show that the effect persists up to 500 kHz. To explain the phenomenon, the effective passivation of surface trap states by mobile carriers is speculated. This, in turn, causes local changes in the NW emission quantum yield (QY). To verify the presence of such mobile charges, both ensemble and single NW bundle electrophoresis experiments are conducted. By investigating subsequent NW rotational and translational dynamics, an estimate for the number of mobile carriers is determined. A lower limit (best case) linear charge density of ～0.45-1.2 mobile electrons per micrometer of the wire is obtained. Apart from self-consistently explaining the field-induced NW emission modulation, the resulting data and subsequent analysis also suggests that the same mobile carriers may be the root cause of NW emission intermittency. Furthermore, given the ubiquity of stray charges, the resulting hypothesis may have additional applicability toward explaining blinking in other systems, a problem of current interest especially within the context of colloidal QDs.