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Intrinsic radiative lifetime derived via absorption cross section of one-dimensional excitons.

ABSTRACT: Intrinsic radiative lifetime is an essential physical property of low-dimensional excitons that represents their optical transition rate and wavefunction, which directly measures the probability of finding an electron and a hole at the same position in an exciton. However, the conventional method that is used to determine this property via measuring the temperature-dependent photoluminescence (PL) decay time involves uncertainty due to various extrinsic contributions at high temperatures. Here, we propose an alternative method to derive the intrinsic radiative lifetime via temperature-independent measurement of the absorption cross section and transformation using Einstein's A-B-coefficient equations derived for low-dimensional excitons. We experimentally verified our approach for one-dimensional (1D) excitons in high-quality 14 × 6 nm(2) quantum wires by comparing it to the conventional approach. Both independent evaluations showed good agreement with each other and with theoretical predictions. This approach opens a promising path to studying low-dimensional exciton physics.

SUBMITTER: Chen S

PROVIDER: S-EPMC3672882 | biostudies-literature | 2013

REPOSITORIES: biostudies-literature

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Intrinsic radiative lifetime derived via absorption cross section of one-dimensional excitons.

Chen Shaoqiang S Yoshita Masahiro M Ishikawa Akira A Mochizuki Toshimitsu T Maruyama Shun S Akiyama Hidefumi H Hayamizu Yuhei Y Pfeiffer Loren N LN West Ken W KW

Scientific reports 20130101

Intrinsic radiative lifetime is an essential physical property of low-dimensional excitons that represents their optical transition rate and wavefunction, which directly measures the probability of finding an electron and a hole at the same position in an exciton. However, the conventional method that is used to determine this property via measuring the temperature-dependent photoluminescence (PL) decay time involves uncertainty due to various extrinsic contributions at high temperatures. Here, ...[more]

PMID: 23736905

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Project description:Optical absorption is the most fundamental optical property characterizing light-matter interactions in materials and can be most readily compared with theoretical predictions. However, determination of optical absorption cross-section of individual nanostructures is experimentally challenging due to the small extinction signal using conventional transmission measurements. Recently, dramatic increase of optical contrast from individual carbon nanotubes has been successfully achieved with a polarization-based homodyne microscope, where the scattered light wave from the nanostructure interferes with the optimized reference signal (the reflected/transmitted light). Here we demonstrate high-sensitivity absorption spectroscopy for individual single-walled carbon nanotubes by combining the polarization-based homodyne technique with broadband supercontinuum excitation in transmission configuration. To our knowledge, this is the first time that high-throughput and quantitative determination of nanotube absorption cross-section over broad spectral range at the single-tube level was performed for more than 50 individual chirality-defined single-walled nanotubes. Our data reveal chirality-dependent behaviors of exciton resonances in carbon nanotubes, where the exciton oscillator strength exhibits a universal scaling law with the nanotube diameter and the transition order. The exciton linewidth (characterizing the exciton lifetime) varies strongly in different nanotubes, and on average it increases linearly with the transition energy. In addition, we establish an empirical formula by extrapolating our data to predict the absorption cross-section spectrum for any given nanotube. The quantitative information of absorption cross-section in a broad spectral range and all nanotube species not only provides new insight into the unique photophysics in one-dimensional carbon nanotubes, but also enables absolute determination of optical quantum efficiencies in important photoluminescence and photovoltaic processes.

Dataset Information

Intrinsic radiative lifetime derived via absorption cross section of one-dimensional excitons.

Publications

Intrinsic radiative lifetime derived via absorption cross section of one-dimensional excitons.

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