High-Temperature Luminescence Quenching of Colloidal Quantum Dots

Abstract

A high luminescence efficiency is an important property of colloidal quantum dots (QDs), and quantum yields higher than 90% have been reported for coreÀshell QDs. 1 High efficiencies are especially important for application of QDs as luminescent biolabels, 2 in QD lasers, 3 in spectral converters for warm white LEDs, 4,5 electroluminescent devices, 6 and solar concentrators. 7 Luminescence efficiencies are strongly temperature-dependent. 8 Extensive temperature-dependent luminescence studies for colloidal QDs have been conducted at cryogenic temperatures (0.3À300 K). 9À15 In this temperature region, interesting effects were observed, including a prolonged lifetime below 20 K related to brightÀdark state splitting, 11,16 thermally activated quenching due to surface defect states, 9,10,17 and temperature antiquenching assigned to a phase transition in the capping layer. 14,15 However, the luminescence properties of QDs above room temperature (RT) are hardly investigated, and yet, for most applications in luminescent devices, the working temperature is higher than 300 K. An interesting example is the recent application of QDs as color converters in warm-white LEDs, 18 in which QDs serve as narrow band red emitters under excitation with blue light from a (In,Ga)N LED. The narrow emission bandwidth renders QDs superior to classical phosphors based on broad band emission from luminescent ions. 19 In high-power LEDs for general lighting applications, the heat generated in the pÀn junction and phosphor converter layer leads to temperatures as high as 150À200°C in the layer applied on top of the blue diode. 20 To avoid these high temperatures, the QD phosphor layer can be placed in a more remote configuration. Still, temperatures in such a configuration are expected to be well above 50°C due to heat dissipation of the QDs themselves (excess energy from converting the blue into red light). Clearly, the quenching of QD luminescence at elevated temperatures is relevant for application of QDs in luminescent devices, and a better insight in the quenching behavior is needed.Despite its importance, research on luminescence temperature quenching above RT is very limited for QDs. It is theoretically expected for a QD to have a very high luminescence quenching temperature (T q ). Three generally accepted mechanisms for thermal quenching involve thermally activated crossover from the excited state to the ground state, multiphonon relaxation, and thermally activated photoionization. The first mechanism is generally depicted in a simple configurational coordinate diagram. 8,21 The energy difference between the minimum * Address correspondence to a.meijerink@uu.nl.Received for review July 18, 2012 and accepted September 14, 2012. Published online 10.1021/nn303217qABSTRACT Thermal quenching of quantum dot (QD) luminescence is important for application in luminescent devices. Systematic studies of the quenching behavior above 300 K are, however, lacking. Here, high-temperature (300À500 K) luminescence studies are reported for highly ef...

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“…Brought to you by | MIT Libraries Authenticated Download Date | 5/13/18 8:01 AM It is a well known fact that the QD emission intensity weakens [25] when strong optical excitation is applied due to issues related to photostability or when the QDs are subjected to high temperatures due to thermal droop, which is the case for the QDs integrated on high-power LEDs. To address this problem, researchers from Samsung proposed the integration of QDs into silica monoliths [26].…”