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Long delays of light in ZnO caused by exciton-polariton propagation
Linköping University, Department of Physics, Chemistry and Biology, Functional Electronic Materials. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Functional Electronic Materials. Linköping University, The Institute of Technology.ORCID iD: 0000-0002-6405-9509
Linköping University, Department of Physics, Chemistry and Biology, Functional Electronic Materials. Linköping University, The Institute of Technology.
2012 (English)In: Physica status solidi. B, Basic research, ISSN 0370-1972, E-ISSN 1521-3951, Vol. 249, no 7, 1307-1311 p.Article in journal (Refereed) Published
Abstract [en]

We study the propagation of exciton-polaritons through bulk ZnO using time-resolved photoluminescence (PL) complemented by time-of-flight measurements of laser pulses. When the photon energy approaches donor bound exciton resonances, substantial time delays in PL light propagation are observed which reach up to 210 ps for a 0.55 mm thick crystal. By comparing results from time-of-flight measurements performed using PL light and laser pulses, the observed delay is shown to be due to the formation of exciton-polaritons and their spectral dispersion. It is also shown that the main contribution to the slow-down effect arises from free exciton-polaritons, whereas bound exciton-polaritons become important only in close vicinity to the corresponding resonances.

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2012. Vol. 249, no 7, 1307-1311 p.
Keyword [en]
excitons; polaritons; slow light; time-of-flight measurements; zinc oxide
National Category
Natural Sciences Condensed Matter Physics
URN: urn:nbn:se:liu:diva-74670DOI: 10.1002/pssb.201147559ISI: 000305966600001OAI: diva2:489928
Available from: 2012-02-03 Created: 2012-02-03 Last updated: 2013-12-16
In thesis
1. Excitonic Effects and Energy Upconversion in Bulk and Nanostructured ZnO
Open this publication in new window or tab >>Excitonic Effects and Energy Upconversion in Bulk and Nanostructured ZnO
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Zinc Oxide (ZnO), a II-VI wurtzite semiconductor, has been drawing enormous research interest for decades as an electronic material for numerous applications. It has a wide and direct band gap of 3.37eV and a large exciton binding energy of 60 meV that leads to intense free exciton (FX) emission at room temperature. As a result, ZnO is currently considered among the key materials for UV light emitting devices with tailored dimensionality and solid state white lighting. Full exploration of ZnO in various applications requires detailed knowledge of its fundamental and materialrelated properties, which remains incomplete. The research work summarized in this thesis addresses a selection of open issues on optical properties of ZnO based on (but not limited to) detailed time-resolved photoluminescence (PL) and magneto-optical studies of various excitonic transitions as specified below.

Papers 1 and 2 analyze recombination dynamics of FX and donor bound excitons (DX) in bulk and tetrapod ZnO with the aim to evaluate contributions of radiative and nonradiative carrier recombination processes in the total carrier lifetime. We show that changes in relative contributions of these processes in “bulk” and near-surface areas are responsible for bi-exponential exciton decays typically observed in these materials. The radiative FX lifetime is found to be relatively long, i.e. >1 ns at 77 K and >14 ns at room temperature. In the case of DX, the radiative lifetime depends on exciton localization. Radiative recombination is concluded to dominate the exciton dynamics in “bulk regions” of high-quality materials. It leads to appearance of a slow component in the decays of no-phonon (NP) FX and DX lines, which also determines the dynamics of the longitudinal optical (LO) phonon-assisted and two-electronsatellite DX transitions. On the other hand, the fast component of the exciton decays is argued to be a result of surface recombination.

Paper 3 evaluates exciton-phonon coupling in bulk and tetrapod ZnO. It is found that, in contrast to bulk ZnO, the NP FX emission in ZnO tetrapods is weak as compared with the LO phonon assisted transitions. We show that the observed high intensity of the FX-1LO emission does not reflect enhanced exciton-phonon coupling in nanostructured ZnO. Instead, it is a result of stronger suppression of the NP FX emission in faceted regions of the tetrapods as revealed from spatially resolved cathodoluminescence (CL) studies. This is attributed to enhanced re-absorption due to multiple internal reflections, which become especially pronounced in the vicinity of the FX resonance.

Effects of exciton-photon coupling on light propagation through the ZnO media are studied in Papers 4 and 5. By employing the time-of-flight spectroscopy, in Paper 4 we demonstrate that the group velocity of laser pulses propagating through bulk ZnO can be slowed down to as low as 2044 km/s when photon energies approach the optical absorption edge of the material. The magnitude of this decrease can be manipulated by changing light polarization. In Paper 5 we show that the observed slow-down is caused by the formation of free exciton-polaritons and is determined by their dispersion. On the other hand, contributions of DX polaritons become important only in the proximity to their corresponding resonances.

Excitonic effects can also be utilized to investigate fundamental properties and defect formation in ZnO. In Paper 6, we employ DX to study magneto-optical properties of the B valence band (B-VB) states as well as dynamics of inter-VB energy relaxation. We show that PL decays of the emissions involving the B-VB holes are faster than that of their counterparts involving the A-VB holes, which is interpreted as being due to energy relaxation of the holes assisted by acoustic phonons. Values of effective Landé g factors for the B-VB holes are also accurately determined. In paper 7, we uncover the origin of a new class of bound exciton lines detected within the nearband-edge region. Based on their magnetic behavior we show that these lines do not stem from DXs bound to either ionized or neutral donors but instead arise from an exciton bound to an isoelectronic center with a hole-attractive local potential.

In Paper 8, DX emissions are used to monitor energy upconversion in bulk and nanorod ZnO. Based on excitation power dependent PL measurements performed with different energies of excitation photons, the physical processes responsible for the upconversion are assigned to two-photon-absorption (TPA) via virtual states and twostep TPA (TS-TPA) via real states. In the former case the observed threshold energy for the TPA process is larger than half of that for one-photon absorption across the bandgap, which can be explained by the different selection rules between the involved optical transitions. It is also concluded that the TS-TPA process occurs via a defect/impurity with an energy level lying within 1.14-1.56 eV from one of the band edges, likely a zinc vacancy.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2014. 57 p.
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1560
National Category
Natural Sciences
urn:nbn:se:liu:diva-102594 (URN)10.3384/diss.diva-102594 (DOI)978-91-7519-464-6 (print) (ISBN)
Public defence
2014-01-31, Planck, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 10:15 (English)
Available from: 2013-12-16 Created: 2013-12-16 Last updated: 2013-12-17Bibliographically approved

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