Abstract

ZnO nanorods (NRs) self-organized into flowers were synthesized at different temperatures ranging from 100°C to 180°C by using the hydrothermal method. The existence of Zn interstitials (Zn(i)) was confirmed by X-ray photoelectron spectroscopy and a larger amount of Zn(i) was found in the ZnO NRs prepared at higher temperatures. A redshift of the emission peak of more than 15 nm was observed for the ZnO NRs under single photon excitation. The nonlinear optical properties of the flower-like ZnO NRs were characterized by using focused femtosecond laser light and strong three-photon-induced luminescence was observed at an excitation wavelength of ~750 nm. More interestingly, a large redshift of the emission peak was observed with increasing excitation intensity, resulting in efficient blue emission with a narrow bandwidth of ~30 nm. It was confirmed that the large redshift originates from the heating of the ZnO NRs to a temperature of more than 800°C and the closely packed ZnO NRs in the flowers play a crucial role in heat accumulation. The stable and efficient three-photon-induced blue emission from such ZnO NRs may find potential applications in the fields of optical display, high-temperature sensors and light therapy of tumors.

Highlights

  • As a semiconductor with wide band gap (3.37 eV) and large exciton binding energy (60 meV), ZnO has attracted great interest in the last two decades due to its potential applications in various fields of science and technology [1,2]

  • The nonlinear optical responses of ZnO nanomaterials have become the focus of many studies because of their potential applications in the field of biophotonics where the use of laser light in the near infrared region is preferred in order to avoid the damage of living tissue

  • We report on the synthesis of Zn interstitials (Zni)-rich ZnO NRs by using a fast hydrothermal method in which three soft templates (PEG, cetyltrimethyl ammonium bromide (CTAB) and TEA) were employed

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Summary

Introduction

As a semiconductor with wide band gap (3.37 eV) and large exciton binding energy (60 meV), ZnO has attracted great interest in the last two decades due to its potential applications in various fields of science and technology [1,2]. With the rapid development in synthesis method and characterization technique, ZnO nanomaterials in different fashions have been intensively and extensively investigated owing to their unique optical, electronic, thermotic, magnetic, and acoustic properties and much attention has been paid to ZnO nanowires or nanorods (NRs) that exhibit many interesting physical properties and great potential in practical application. This kind of one-dimensional nanomaterials is considered as a potential candidate for making sophisticated optoelectronic devices. The blue emission originated from the cooperation of the three-photon-induced luminescence (3PL) and the significant heat accumulation effect existing in the flower-like ZnO NRs

Experimental detail and numerical method
PL spectra of the ZnO NRs under single photon excitation
Nonlinear optical properties of the ZnO NRs
Physical mechanism for the redshift of the MPL
Heat accumulation effect
Physical mechanism for the 3PL of the ZnO NRs
Conclusion
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