The Enabling Role of Surface Passivation in Visible Photoluminescence from Si Nanoparticles

1993 ◽  
Vol 318 ◽  
Author(s):  
A.A. Seraphin ◽  
E. Werwa ◽  
L.A. Chiu ◽  
K.D. Kolenbrander

ABSTRACTSilicon nanocrystallites have been studied in a variety of passivating environments to study the role of surface passivation in visible light emission from the particles. Thin films of Si nanocrystallites have been deposited by a laser ablation supersonic expansion technique. The films show significant room temperature photoluminescence (PL) behavior only after processing to achieve surface passivation. Passivation effects on light emission are studied through PL emission spectroscopy on clusters in the gas phase, as well as films in a variety of passivating media. The intensity of PL emission seems to scale with the extent of surface passivation, but the specific nature of the passivating species is not critical in defining the wavelength of emitted light.

1995 ◽  
Vol 405 ◽  
Author(s):  
A. A. Seraphin ◽  
S.-T. Ngiam ◽  
K. D. Kolenbrander

AbstractThe visible photoluminescence from thin films of silicon nanocrystallites produced by a pulsed laser ablation supersonic expansion source has been studied to determine the role of particle surface and size in the emission behavior. Variation of nanocrystallite size and surface through a variety of chemical treatments and processing steps has shown that the visible emission can be explained using only a simple quantum confinement model. Particle size has been reduced through a series of acid etch and reoxidation cycles and compared to sample emission wavelength. The role of surface species in determining emission behavior has been studied by chemically altering the surfaces and comparing their surface properties as determined by x-ray photoelectron spectroscopy to their photoluminescence behavior. Nanocrystallite size controls the emission energy, while surface passivation only determines emission intensity, through control of excited carrier recombination pathways.


1994 ◽  
Vol 358 ◽  
Author(s):  
A.A. Seraphin ◽  
F.J. Aranda ◽  
E. Werwa ◽  
D.V.G.L.N. Rao ◽  
K.D. Kolenbrander

ABSTRACTDegenerate four-wave mixing with picosecond pulses at 532 nm has been used to study the third-order nonlinear optical susceptibility (x(3)) for a series of passivated thin films of silicon nanocrystallites. A pulsed laser ablation supersonic expansion source of isolated silicon nanocrystallites was used to deposit thin films onto inert substrates. These films were subsequently passivated using chemical etches or oxidation steps. We observe a strong dependence of the measured x(3) as a function of the degree of passivation, indicating the fundamental importance of the surface of the nanocrystallite in enabling the nonlinear optical behavior. Systems providing more complete passivation were found to have greatly enhanced X(3) behavior when compared to poorly passivated systems. Surface passivation is also shown to be critical to the visible photoluminescence behavior of the thin films, as poorly passivated nanocrystallites exhibit very weak light emission, while well passivated systems show efficient emission. In both cases, the passivation controls the recombination pathways of excited carriers and determines the material's optical properties.


2008 ◽  
Vol 8 (1) ◽  
pp. 366-373 ◽  
Author(s):  
M.-Y. Tsai ◽  
J.-J. Chiu ◽  
S.-F. Horng ◽  
C. C. Chi ◽  
T.-P. Perng

Si nanocrystallites of various sizes and oxygen-containing Si nanoparticles with different oxygen contents were prepared by vapor condensation. The Si nanocrystallites showed a visible light emission from 500 nm to 900 nm with the peak at 800 nm, and the intensity of photoluminescence increased with decreasing the particle size. This photoluminescence observed in vacuum could be quenched by air and hydrogen, and reappeared after the sample chamber was evacuated. The oxygen-containing Si nanoparticles consisting mainly of Si oxide were amorphous and had an average particle size of approximately 20 nm. Increasing the oxygen content of nanoparticles caused a blueshift of the absorption edge in the transmission spectra. A blue-green photoluminescence with two peaks at 500 nm and 800 nm was observed from these oxygen-containing Si nanoparticles. The luminescence intensity increased with the oxygen content of nanoparticles, and was very sensitive to the ambient atmosphere. Much lower intensity was observed in air, but higher intensity could be recovered in vacuum. Surface states and oxygen-induced luminescent centers were proposed to be responsible for the photoluminescence from the Si nanocrystallites and oxygen-containing Si nanoparticles, respectively. The reversible ambient effect in both cases could be explained by surface charge redistribution during the gas adsorption and desorption processes.


AIP Advances ◽  
2017 ◽  
Vol 7 (5) ◽  
pp. 055109 ◽  
Author(s):  
A. A. González-Fernández ◽  
J. Juvert ◽  
M. Aceves-Mijares ◽  
C. Dominguez-Horna

1998 ◽  
Vol 536 ◽  
Author(s):  
S. Miyazaki ◽  
K. Shiba ◽  
N. Miyoshi ◽  
K. Etoh ◽  
A. Kohno ◽  
...  

AbstractHemispherical silicon quantum dots (QDs) have been self-assembled with an areal density as high as ~2−1011 cm−2 on SiO2/Si(100) and quartz substrates by controlling the early states of low pressure chemical vapor deposition (LPCVD) of pure silane. It is found that, for the thermally-oxidized Si QDs, when the mean Si dot height is decreased from 6.3 nm to 1~2 nm, the photoluminescence (PL) peak energy is increased from 1.2 to 1.4 eV at room temperature while the optical absorption edge determined by photothermal deflection spectroscopy is shifted from 1.9 to 2.5 eV. In addition to the observed Stokes shift as large as 0.7−1.1 eV, a weak temperature dependence of the broad luminescence band and non-exponential luminescence decay with a mean life time of sub-msec even at room temperature suggest that localized, radiative recombination centers existing presumably in the SiO2/Si dot interface are responsible for the efficient PL from the Si QDs. From the change in room temperature PL by SiO2 thinning and removal in a dilute HF solution, it is demonstrated that the surface passivation of Si QDs plays an important role for the efficient light emission at room temperature.


1995 ◽  
Vol 405 ◽  
Author(s):  
A. Thilderkvist ◽  
J. Michel ◽  
S.-T. Ngiam ◽  
L. C. Kimerling ◽  
K. D. Kolenbrander

AbstractStrong room temperature photoluminescence emission from thin films of Er nanoparticles embedded in a matrix of silicon is reported. The Er nanoparticles were produced by a pulsed laser ablation supersonic expansion technique. After a heat treatment at 500°C in an Ar-atmosphere, intense Er-related luminescence appears at λ = 1.54 gim, characteristic of intra-4f emission from Er3÷. Only a 50% reduction in photoluminescence intensity is observed as the temperature increases from 4 K to 300 K. A photocarrier mediated process is responsible for the excitation of the optically active Er-centers.


2015 ◽  
Vol 1107 ◽  
pp. 308-313
Author(s):  
Sib Krishna Ghoshal ◽  
M.R. Sahar ◽  
R. Arifin ◽  
M.S. Rohani ◽  
K. Hamzah

Tuning the visible emission of Si nanomaterials by modifying their size and shape is one of the key issue in optoelectronics. The observed optical gain in Si-nanoclusters (NCs) has given further impulse to nanosilicon research. We develop a phenomenological model by combining the effects of surface passivation, exciton states and quantum confinement (QC). The size and passivation dependent band gap, oscillator strength, radiative lifetime and photoluminescence (PL) intensity for NCs with diameter ranging from 1.0 to 6.0 nm are presented. By controlling a set of fitting parameters, it is possible to tune the optical band gap, PL peak and intensity. In case of pure clusters, the band gap is found to decrease with increasing NC size. Furthermore, the band gap increases on passivating the surface of the cluster with hydrogen and oxygen respectively in which the effect of oxygen is more robust. Both QC and surface passivation in addition to exciton effects determine the optical and electronic properties of silicon NCs. Visible luminescence is due to radiative recombination of electrons and holes in the quantum-confined NCs. The role of surface states on the band gap as well as on the HOMO-LUMO states is also examined and a correlation is established. Our results are in conformity with other observations. The model can be extended to study the light emission from other nanostructures and may contribute towards the development of Si based optoelectronics.


2020 ◽  
Author(s):  
Bingbing Ding ◽  
Liangwei Ma ◽  
Zizhao Huang ◽  
Xiang Ma ◽  
He Tian

<p>The trace impurities in pure organic phosphors were always ignored because the ultra-low content impurities were considered to hardly affect the luminescent properties. Evidences from corresponding reports and research have shown that impurities may greatly affect room temperature phosphorescence (RTP) in some crystalline compounds. To date, very few literatures have clearly study the role of impurities in RTP because of the difficulty in the separation and structure identification of impurities. Also no reports have focused on utilizing trace impurities to form new strategies for efficient RTP.</p> <p>For the first time, an impurity was isolated from 1-(4-bromophenyl)-1<i>H</i>-imidazole (1BBI) and structural identified, which was proved to be the key to RTP in 1BBI crystal. Neither purified impurity nor 1BBI matrix shown any detectable RTP. The impurity could light up the unusual ultralong RTP in matrix even at <b>0.01 mol%</b> content. Inspired by impurity/matrix phosphorescence, a trace-ingredient-mediated bicomponent strategy was introduced for high phosphorescence quantum yield (QY, up to 74.2%) and extralong lifetime (up to 430 ms).</p><p><b>Research Highlights of this work are including</b></p><p><b>1. </b><b>The study of impurities in organic luminescent materials, including phosphorescent materials, is rarely reported due to the great difficulty of separation, purification</b><b> and structure characterization. This work not only separated, purified and structure identified the trace impurity in the system but also confirmed the fact that the impurity engenders the RTP. And the corresponding mechanism was proposed as well.</b></p><p><b>2. </b><b>Inspired by the role of impurities in RTP, this work proposed an effective strategy for the design and preparation of persistent organic RTP based on active ingredient incorporation. Seven compounds were screened out to conduct the bicomponent RTP system and achieved bright RTP with high QY (up to 74.2%) and extra-long lifetime (up to 430 ms)) RTP with tunable colors.</b></p><p><b>3. </b><b>Combining the dual emission of blue fluorescence and yellow phosphorescence, a bicomponent system achieved a bright white-light emission, which shows its outstanding application potential.</b></p><p> The design concept and strategy of this work supplies an efficient approach to develop RTP by simply mixing the matrix with a trace amount of active ingredients. And the trace-ingredient-mediated bicomponent system is preferred for its high efficiency, color-tunable, low cost and easy to prepare properties, which will make important sense for facilely developing organic persistent RTP materials. This work will not only lead to a new understanding of persistent organic RTP but also develop a facile and effective strategy for RTP afterglow materials.<br></p>


2020 ◽  
Author(s):  
Bingbing Ding ◽  
Liangwei Ma ◽  
Zizhao Huang ◽  
Xiang Ma ◽  
He Tian

<p>The trace impurities in pure organic phosphors were always ignored because the ultra-low content impurities were considered to hardly affect the luminescent properties. Evidences from corresponding reports and research have shown that impurities may greatly affect room temperature phosphorescence (RTP) in some crystalline compounds. To date, very few literatures have clearly study the role of impurities in RTP because of the difficulty in the separation and structure identification of impurities. Also no reports have focused on utilizing trace impurities to form new strategies for efficient RTP.</p> <p>For the first time, an impurity was isolated from 1-(4-bromophenyl)-1<i>H</i>-imidazole (1BBI) and structural identified, which was proved to be the key to RTP in 1BBI crystal. Neither purified impurity nor 1BBI matrix shown any detectable RTP. The impurity could light up the unusual ultralong RTP in matrix even at <b>0.01 mol%</b> content. Inspired by impurity/matrix phosphorescence, a trace-ingredient-mediated bicomponent strategy was introduced for high phosphorescence quantum yield (QY, up to 74.2%) and extralong lifetime (up to 430 ms).</p><p><b>Research Highlights of this work are including</b></p><p><b>1. </b><b>The study of impurities in organic luminescent materials, including phosphorescent materials, is rarely reported due to the great difficulty of separation, purification</b><b> and structure characterization. This work not only separated, purified and structure identified the trace impurity in the system but also confirmed the fact that the impurity engenders the RTP. And the corresponding mechanism was proposed as well.</b></p><p><b>2. </b><b>Inspired by the role of impurities in RTP, this work proposed an effective strategy for the design and preparation of persistent organic RTP based on active ingredient incorporation. Seven compounds were screened out to conduct the bicomponent RTP system and achieved bright RTP with high QY (up to 74.2%) and extra-long lifetime (up to 430 ms)) RTP with tunable colors.</b></p><p><b>3. </b><b>Combining the dual emission of blue fluorescence and yellow phosphorescence, a bicomponent system achieved a bright white-light emission, which shows its outstanding application potential.</b></p><p> The design concept and strategy of this work supplies an efficient approach to develop RTP by simply mixing the matrix with a trace amount of active ingredients. And the trace-ingredient-mediated bicomponent system is preferred for its high efficiency, color-tunable, low cost and easy to prepare properties, which will make important sense for facilely developing organic persistent RTP materials. This work will not only lead to a new understanding of persistent organic RTP but also develop a facile and effective strategy for RTP afterglow materials.<br></p>


Crystals ◽  
2020 ◽  
Vol 10 (5) ◽  
pp. 351
Author(s):  
Lukas Spindlberger ◽  
Johannes Aberl ◽  
Antonio Polimeni ◽  
Jeffrey Schuster ◽  
Julian Hörschläger ◽  
...  

While light-emitting nanostructures composed of group-IV materials fulfil the mandatory compatibility with CMOS-fabrication methods, factors such as the structural stability of the nanostructures upon thermal annealing, and the ensuing photoluminescence (PL) emission properties, are of key relevance. In addition, the possibility of improving the PL efficiency by suitable post-growth treatments, such as hydrogen irradiation, is important too. We address these issues for self-assembled Ge quantum dots (QDs) that are co-implanted with Ge ions during their epitaxial growth. The presence of defects introduced by the impinging Ge ions results in pronounced PL-emission at telecom wavelengths up to room temperature (RT) and above. This approach allows us to overcome the severe limitations of light generation in the indirect-band-gap group-IV materials. By performing in-situ annealing, we demonstrate a high PL-stability of the defect-enhanced QD (DEQD) system against thermal treatment up to 600 °C for at least 2 h, even though the Ge QDs are structurally affected by Si/Ge intermixing via bulk diffusion. The latter, in turn, allows for emission tuning of the DEQDs over the entire telecom wavelength range from 1.3 µm to 1.55 µm. Two quenching mechanisms for light-emission are discussed; first, luminescence quenching at high PL recording temperatures, associated with the thermal escape of holes to the surrounding wetting layer; and second, annealing-induced PL-quenching at annealing temperatures >650 °C, which is associated with a migration of the defect complex out of the QD. We show that low-energy ex-situ proton irradiation into the Si matrix further improves the light emission properties of the DEQDs, whereas proton irradiation-related optically active G-centers do not affect the room temperature luminescence properties of DEQDs.


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