Abstract

We describe a novel technique for measuring carrier dynamics in solid-state optical materials based on photomodulated reflectivity (PMR) and, as an example, apply it to a study of an InGaN/GaN multi-quantum-well (QW) structure grown on a c-plane sapphire substrate. The technique is a form of frequency modulation spectroscopy and relies on probing changes in refractive index induced by fluctuations in free-carrier density during optical excitation. We show that it is possible to accurately determine both carrier density and lifetime, independent of any photoluminescence (PL) measurement and with no knowledge of the incident, or fraction of absorbed, laser power, quantities that can give rise to considerable uncertainties in PL studies. We demonstrate that such uncertainties can lead to an order of magnitude underestimation of the total photogenerated carrier density and compromised accuracy in determining carrier lifetime. We determine, by a comparison of the two techniques, PMR and PL, the nonradiative Shockley–Reed–Hall (SRH), radiative (excitonic), and nonradiative Auger-related coefficients (from the standard ABC model). We find marked differences in the carrier-density-dependent lifetime, determined from PMR, translate to significant differences in the SRH and excitonic coefficients, which we believe relate to the more accurate determination of carrier densities in PMR than in PL. We also find evidence from the PMR for a change in effective mass of the photoexcited carriers with excitation intensity, which points to a complex localization/delocalization mechanism, likely facilitated by random fluctuations in indium content and QW width, consistent with previous findings by independent methods.

Highlights

  • Optical-based modulation spectroscopy lies within a family of techniques that have been developed over many decades to study materials’ properties

  • We report the development of an optical approach to determine the free carrier dynamics in light-emitting diodes (LEDs) material systems based on frequency-resolved spectroscopy

  • There is no widely accepted origin for Article this effect, reports based on PL tend to point to Auger recombination and/or carrier delocalization as the possible causes.[30−32] In the following frequency-resolved experiments we observed no roll-off of the PL in the kHz−MHz regime, as would be expected if there was a thermal contribution to this efficiency reduction, so we believe the external quantum efficiency (EQE) quenching in our experiment to be the same process as that reported widely for this material system

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Summary

Introduction

Optical-based modulation spectroscopy lies within a family of techniques that have been developed over many decades to study materials’ properties.

Results
Conclusion
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