Unconventional photoluminescence upconversion from PbS quantum dots

Fernée, Mark J.; Jensen, Peter; Rubinsztein‐Dunlop, Halina

doi:10.1063/1.2760140

Cited by 25 publications

(23 citation statements)

References 18 publications

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“…The observed continuity of the PL signal intensity between the Stokes and the anti‐Stokes side of the spectra means that the anti‐Stokes process is as efficient as the Stokes one. This is similar to observations made on II–VI and III–V quantum dots and bulk GaN ASPL …”

Section: Resultssupporting

confidence: 91%

Anti‐Stokes Photoluminescence of Monolayer WS₂

Pierret

Tornatzky

Maultzsch

2019

Physica Status Solidi (b)

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Anti‐Stokes photoluminescence excitation of a WS2 monolayer flake between 10 and 300 K is reported herein. Even with continuous‐wave lasers at low power, the emission of the exciton at excitation 100 meV below its emission energy at room temperature is observed. A mechanism which involves the trions as the intermediate state is proposed, leading to an efficient up‐conversion process. In addition, it is demonstrated that phonons are the source of the additional energy needed by the system. Overall, the results provide evidence that anti‐Stokes luminescence in transition metal dichalcogenides is very efficient.

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Section: Resultssupporting

confidence: 91%

Anti‐Stokes Photoluminescence of Monolayer WS₂

Pierret

Tornatzky

Maultzsch

2019

Physica Status Solidi (b)

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“…4a, λ exc > 590 nm. A similar observation was reported recently for PbS QDs 25. The gradual change in the band shape suggests that the physical process involved in the QD emission is the same throughout the whole range of excitation energies.…”

Section: Phonon‐assisted Anti‐stokes Photoluminescence In Nanocrystsupporting

confidence: 88%

“…However, it happens that, most likely, the bare exciton level structure described above is not directly related to the PL up‐conversion effect. Experimentally, the blue (anti‐Stokes) shift between the ASPL peak and E abs does not significantly depend upon the QD size when the excitation photon energy is chosen proportionally to the absorption peak energy (which depends upon the size) 17–26. This is at variance with the strong size dependence of Δ E .…”

Section: Phonon‐assisted Anti‐stokes Photoluminescence In Nanocrystmentioning

confidence: 84%

“…So far, a record efficiency of 99% has been observed in a GaAs/GaInP double heterostructure only by decreasing temperature down to 100 K 12. These advantages along with the numerous recent reports on efficient ASPL 17–26 motivated us to gain insight into the feasibility of the proposed approach and requirements for achieving net laser cooling using one particular type of semiconductor nanostructures, namely nanocrystal quantum dots (QDs) fabricated via colloidal chemistry.…”

Section: Introductionmentioning

confidence: 99%

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Anti‐Stokes cooling in semiconductor nanocrystal quantum dots: A feasibility study

Rakovich

Donegan

Vasilevskiy

et al. 2009

Physica Status Solidi (a)

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Multicolor luminescent films have great potential for use in optoelectronics, solid‐state light‐emitting materials, and optical devices. This work describes a systematic investigation of the ordered assembly of two‐ (blue/green, blue/orange, red/blue, red/green) and three‐color (blue/red/green) light‐emitting ultrathin films (UTFs) by using different photofunctional anions [bis(N‐methylacridinium)@polyvinylsulfonate ion pairs and anionic derivatives of poly(p‐phenylene), poly(phenylenevinylene), and poly(thiophene)] and Mg‐Al‐layered double hydroxide nanosheets as building blocks. The rational combination of luminescent components affords precise control of the emission wavelengths and intensity, and multicolored luminescent UTFs can be precisely tailored covering most of the visible spectral region. The assembly process of the UTFs and their luminescence properties, as monitored by UV–vis absorption and fluorescence spectroscopy, resulted in a gradual change in luminescence color in the selected light‐emitting spectral region upon increasing the number of deposition cycles. X‐ray diffraction demonstrates that the UTFs are periodic layered structures involving heterogeneous superlattices associated with individual photoactive anion–LDH units. These UTFs also exhibit well‐defined multicolor polarized fluorescence with high polarization anisotropy, and the emissive color changes with polarization direction. Therefore, this work provides a way of fabricating heterogeneous UTFs with tunable‐color luminescence as well as polarized multicolor emission, which have potential applications in the areas of light displays and optoelectronic devices.

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“…There are some typical schemes, e.g., those based on phonon-assisted processes [17][18][19][20], and on multiphoton processes [21][22][23]. Recently, Fernée et al reported that the up-conversion range is greatly widened by an unusually-large dephasing rate in a colloidal solution of quantum dots [24]. The up-conversion in the present work is essentially distinguished from the previous ones in that it is the PL from the exciton-light coupled state with a higher exciton-light coupled mode.…”

mentioning

confidence: 99%

Upconverted photoluminescence induced by radiative coupling between excitons

2016

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We propose an unconventional scheme of photoluminescence in a semiconductor thin film, where the nonlocal correlation between an excitonic wave and a light wave prominently enhances the exciton-light coupling beyond the long-wavelength approximation (the so-called excitonic superradiance regime). On the basis of the developed method extending input-output theory, we elucidate atypical photoluminescence effects due to the strong wave-wave correlation. In particular, the upconverted photoluminescence based on the coherent superposition of excitons is found to be highly efficient, i.e., it can be realized by weak pumping without auxiliary systems such as cavities or photonic antennas. 71.36.+c, 42.50.Nn Photoluminescence (PL) is one of the fundamental phenomena arising from light-matter coupling, and has been extensively utilized for monitoring the structure of the electronic levels in materials [1]. PL spectroscopy provides the essential information of matter systems, such as the structure of the levels and oscillator strengths of electronic excited states after reaching quasiequilibrium. On the other hand, PL is also important for observing the interplay scheme between light and electronic systems. A representative example is PL reflecting the dispersion relation of polaritons and not the thermal equilibrium for bare excitons [2][3][4]. In order to access polaritons by photon emission, photons have to be emitted before the exciton-photon coupling is "dephased", or the excitations relax to quasi-equilibrium. Then, it is necessary to consider polariton accumulation at the bottleneck of the decay [2], or confine the electronic system in high-density photons [5][6][7][8].Recently, another scheme that allows PL to access exciton-light coupled modes has been demonstrated in simple semiconductor thin films [9]. When the film thickness is in the nano-to-bulk crossover regime (a few hundred nanometers), the exciton-light coupling is extremely enhanced by the nonlocal correlation between a light wave and an excitonic center-of-mass (c.m.) wave [10][11][12][13]. Note that the resultant exciton-light coupled state should be distinguished from polaritons because it exhibits an ultrafast radiative decay exceeding the polariton formation, and is in the so-called excitonic superradiance regime [14][15][16]. Such a strong coupling beyond the long-wavelength approximation (LWA) leads to unprecedented PL properties. Actually, photon emission simultaneously occurs from more than one exciton-light coupled mode including optically-forbidden ones [9].Here, we focus on a unique feature of the beyond the LWA regime; there exists strong coupling between the different c.m. states of excitons via radiation that causes quantum superposition of these states. The purpose of * Electronic address: matsuda@pe.osakafu-u.ac.jp † Electronic address: ishi@pe.osakafu-u.ac.jp this paper is to theoretically demonstrate that the control of the superposition provides unconventional and functional aspects of PL properties. In particular, remarkable up-...

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Unconventional photoluminescence upconversion from PbS quantum dots

Cited by 25 publications

References 18 publications

Anti‐Stokes Photoluminescence of Monolayer WS₂

Anti‐Stokes Photoluminescence of Monolayer WS₂

Anti‐Stokes cooling in semiconductor nanocrystal quantum dots: A feasibility study

Upconverted photoluminescence induced by radiative coupling between excitons

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Unconventional photoluminescence upconversion from PbS quantum dots

Cited by 25 publications

References 18 publications

Anti‐Stokes Photoluminescence of Monolayer WS2

Anti‐Stokes Photoluminescence of Monolayer WS2

Anti‐Stokes cooling in semiconductor nanocrystal quantum dots: A feasibility study

Upconverted photoluminescence induced by radiative coupling between excitons

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Product

Resources

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Anti‐Stokes Photoluminescence of Monolayer WS₂

Anti‐Stokes Photoluminescence of Monolayer WS₂