We are reporting ultrafast charge carrier and charge transfer dynamics of the CdTe quantum dot (QD) and type II CdTe/CdS core-shell QD materials with different shell (CdS) thicknesses. Herein, we have synthesized CdTe and CdTe/CdS core-shell quantum dots by using 3-mercaptopropionic acid as a capping agent. Steady state absorption and emission studies confirmed successful synthesis of CdTe QD and CdTe/CdS core-shell QD materials. Time-resolved emission studies indicate a longer emission lifetime of the CdTe/CdS core-shell as compared to CdTe QD materials, where in both cases only CdTe gets excited. We have carried out femtosecond transient absorption studies of these QD and core-shell materials by exciting them with 400 nm laser light and monitoring the transients in the visible to near-IR region to study charge carrier and charge transfer dynamics in the ultrafast time scale. On laser excitation, electron-hole pairs are generated which are confirmed by induced absorption signal for the charge carriers in the visible and near-IR region and an immediate bleach at excitonic position for both QD and QD core-shell. The carrier relaxation was found to be slower and the carrier lifetime was found to be longer in the QD core-shell as compared to the QD indicating charge transfer from core to shell. Carrier quenching studies have been carried out for both CdTe and CdTe/CdS by using benzoquinone (BQ, electron quencher) and Pyridine (Py, hole quencher) to assign the different relaxation processes. Details about the relaxation of hot carriers and the quenching effect on the relaxation dynamic of the charge carriers have been discussed for both QD and core-shell nanostructures.
Nanocatalysis has been a growing field over the past few decades with significant developments in understanding the surface properties of nanocatalysts. With recent advances in synthetic methods, size, shape and composition of the nanoparticles can be controlled in a well defined manner which facilitates achieving selective reaction products in multipath reactions. Nanoparticles with specific exposed crystal facets can have different reactivity than other facets for reaction intermediates, which favours selective pathways during the course of reaction. Heterogeneous catalysts have been studied extensively; nano‐sized metal particles are absorbed on mesoporus supports, facilitating access to the large surface area of the nanoparticles and hence exposure of more catalytic sites. Photocatalysis is attractive area of catalysis, in which photoinduced charge carriers are used for a variety of catalytic applications. More interestingly, clean and renewable liquid fuels energy sources such as hydrogen and methyl alcohol can be generated using photocatalysts through water splitting and CO2 reduction, respectively. Herein, we highlight the progress of nanocatalysis through metal, bimetallic nanoparticle, metal‐semiconductor hybrid nanostructures and oxide nanoparticles for various reactions.
We report the ultrafast charge carrier relaxation dynamics of mercaptopropionic acid capped CdTe quantum dot (QD) using femtosecond transient absorption spectroscopy by exciting the particles with 400 nm laser light and monitoring the transients in the visible to near IR region. Cooling dynamics and population dynamics in different quantized states of the charge carriers were monitored by following the growth kinetics of the bleach at different excitonic positions. The cooling time second and first excitonic states were found to be 150 fs and 500 fs, respectively, which increases non-linearly with its size. Defect states of QD surface play an important role in the cooling dynamics of the charge carriers. Quenching studies have been carried out to find out cooling and trapping dynamics of the individual charge carriers. Electron and hole cooling time were measured to be 700 fs and 150 fs for the first excitonic state using quenchers. Trapping dynamics of electron and hole have been determined by monitoring transient signal at 1000 nm and by using hole and electron quencher, respectively. Electron and hole trapping times have been found to be 700 fs and 1 ps, respectively, in CdTe QD.
We report synthesis and ultrafast charge transfer dynamics of photoexcited CdTe quantum dots (QDs) decorated on graphene. We have synthesized CdTe QD particles of 2.2 nm sizes with first exciton (1S3/2-1Se) band ∼450 nm and then decorated the QD particles on graphene which has been confirmed by HRTEM studies. The CdTe QD decorated graphene has been named as G-CdTe. Steady state emission studies revealed that on the graphene surface CdTe emission gets quenched drastically which indicates the charge transfer from photoexcited CdTe to graphene. To unravel the charge transfer dynamics in ultrafast time scale we have carried out femtosecond transient absorption studies by exciting the CdTe QD particles and monitoring the transients in the visible to near-IR region. Transient absorption studies indicate that exciton recombination time (as monitored the exciton bleach) of pure CdTe QD takes place within 50 ps; however, on graphene the surface exciton recombination time was found to be much longer (>1 ns). Our studies clearly indicate that charge separation of G-CdTe composite materials drastically improves as compared to that CdTe QD.
We have synthesized thiol-capped CdSe/ZnTe quantum dot core−shell nanostructures by colloidal methods, have characterized them by steady-state absorption and photoluminescence (PL) spectroscopy and further confirmed by high resolution transmission electron microscopy and X-ray diffraction measurements. Clear red shift on shell formation was observed in optical absorption and photoluminescence studies. Time-resolved emission studies indicate longer emission lifetime of CdSe/ZnTe core−shell as compared to CdSe QD material where in both cases only CdSe gets excited, which indicates spatial charge separation in type-II core−shell. Ultrafast photoinduced charge transfer dynamics in type-II CdSe/ZnTe donor−acceptor core−shell were studied in real-time using femtosecond broadband pump−probe spectroscopy. Our transient absorption studies suggests that on photoexcitation core−shell hole transfer from CdSe core to ZnTe shell takes place in pulse-width limited time scale as evidenced by an increase in cooling dynamics of the charge carriers from 150 fs for CdSe to 300 fs for thickest CdSe/ZnTe core−shell. Increase in cooling dynamics in core−shell has been explained due to decoupling of electron and hole in photoexcited core−shell. Trapping dynamics play a major role in the excited dynamics of the photoexcited charge carriers of quantum dot materials. Bleach recovery kinetics of the photoexcited QD materials fitted multi-exponentially where 2.5 ps (first component) has been attributed to the electron trapping dynamics and the longer components (30−50 ps and >400 ps) attributed to the charge recombination dynamics.
Herein, we report the synthesis of aqueous CdTe/CdSe type-II core-shell quantum dots (QDs) in which 3-mercaptopropionic acid is used as the capping agent. The CdTe QDs and CdTe/CdSe core-shell QDs are characterized by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HR-TEM), steady-state absorption, and emission spectroscopy. A red shift in the steady-state absorption and emission bands is observed with increasing CdSe shell thickness over CdTe QDs. The XRD pattern indicates that the peaks are shifted to higher angles after growth of the CdSe shell on the CdTe QDs. HR-TEM images of both CdTe and CdTe/CdSe QDs indicate that the particles are spherical, with a good shape homogeneity, and that the particle size increases by about 2 nm after shell formation. In the time-resolved emission studies, we observe that the average emission lifetime (τ(av)) increases to 23.5 ns for CdTe/CdSe (for the thickest shell) as compared to CdTe QDs (τ(av) =12 ns). The twofold increment in the average emission lifetime indicates an efficient charge separation in type-II CdTe/CdSe core-shell QDs. Transient absorption studies suggest that both the carrier cooling and the charge-transfer dynamics are affected by the presence of traps in the CdTe QDs and CdTe/CdSe core-shell QDs. Carrier quenching experiments indicate that hole traps strongly affect the carrier cooling dynamics in CdTe/CdSe core-shell QDs.
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