Malko, Anton V.

Permanent URI for this collectionhttps://hdl.handle.net/10735.1/3870

Anton Malko is a Professor of Physics and head of the Optics and Ultrafast Spectroscopy Laboratory. Among his research interests are

  • Experimental Condensed Matter
  • Optical Spectroscopy of Nanoparticles
  • Optical Properties of Semiconductors
  • Nano-optics
  • Non-linear optics
  • Femtosecond Spectroscopy
  • Time-resolved Photoluminescence
  • Nanostructured Solar Cells
  • Energy Transfer in Nanoscopic Systems
  • Quantum Optics
For more information about Dr. Malko see his departmental Home page, his Research Explorer page as well as the Optics and Ultrafast Spectroscopy Laboratory website.

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Recent Submissions

Now showing 1 - 8 of 8
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    Using Shape to Turn off Blinking for Two-Colour Multiexciton Emission in CdSe/CdS Tetrapods
    (2017-05-12) Mishra, Nimai; Orfield, Noah J.; Wang, Feng; Hu, Zhongjian; Krishnamurthy, Sachidananda; Malko, Anton V.; Casson, Joanna L.; Htoon, Han; Sykora, Milan; Hollingsworth, Jennifer A.; Krishnamurthy, Sachidananda; Malko, Anton V.
    Semiconductor nanostructures capable of emitting from two excited states and thereby of producing two photoluminescence colours are of fundamental and potential technological significance. In this limited class of nanocrystals, CdSe/CdS core/arm tetrapods exhibit the unusual trait of two-colour (red and green) multiexcitonic emission, with green emission from the CdS arms emerging only at high excitation fluences. Here we show that by synthetic shape-tuning, both this multi-colour emission process, and blinking and photobleaching behaviours of single tetrapods can be controlled. Specifically, we find that the properties of dual emission and single-nanostructure photostability depend on different structural parameters-arm length and arm diameter, respectively-but that both properties can be realized in the same nanostructure. Furthermore, based on results of correlated photoluminescence and transient absorption measurements, we conclude that hole-trap filling in the arms and partial state-filling in the core are necessary preconditions for the observation of multiexciton multi-colour emission.
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    Propagation and Absorption of Light in Planar Dielectric Waveguides with Two-Dimensional Semiconductors
    (Optical Soc Amer, 2017-09-12) Gartstein, Yuri N.; Malko, Anton V.; 0000 0001 2678 9765 (Malko, AV); Gartstein, Yuri N.; Malko, Anton V.
    Strong optical responses of atomically thin two-dimensional (2D) semiconductors make them attractive candidates for integration into various photonic and optoelectronic structures. We discuss some fundamental effects of such integration into planar dielectric waveguides by demonstrating that a substantial modification of the spectrum of waveguide modes can occur due to high in-plane polarizability of 2D layers. Our calculations illustrate both the conceptual possibilities associated with sharp excitonic resonances as well as the results obtained with the experimentally assessed polarizability of monolayer MoS2 over a broad spectral range. We point out that waveguide structures could also enable the tunable absorption by 2D semiconductors of the light that propagates along them, a modality quite different from the traditional light harvesting geometry.
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    Energy Transfer from Colloidal Nanocrystals to Strongly Absorbing Perovskites
    (Royal Society of Chemistry, 2018-06-01) Cabrera, Yasiel; Rupich, Sara M.; Shaw, Ryan; Anand, Benoy; Villa, Manuel de Anda; Rahman, Rezwanur; Dangerfield, Aaron; Gartstein, Yuri N.; Malko, Anton V.; Chabal, Yves J.; 0000-0002-6435-0347 (Chabal, YJ); Cabrera, Yasiel; Rupich, Sara M.; Shaw, Ryan; Anand, Benoy; Villa, Manuel de Anda; Rahman, Rezwanur; Dangerfield, Aaron; Gartstein, Yuri N.; Malko, Anton V.; Chabal, Yves J.
    Integration of colloidal nanocrystal quantum dots (NQDs) with strongly absorbing semiconductors offers the possibility of developing optoelectronic and photonic devices with new functionalities. We examine the process of energy transfer (ET) from photoactive CdSe/ZnS core/shell NQDs into lead-halide perovskite polycrystalline films as a function of distance from the perovskite surface using time-resolved photoluminescence (TRPL) spectroscopy. We demonstrate near-field electromagnetic coupling between vastly dissimilar excitation in two materials that can reach an efficiency of 99% at room temperature. Our experimental results, combined with electrodynamics modeling, reveal the leading role of non-radiative ET at close distances, augmented by the waveguide emission coupling and light reabsorption at separations >10 nm. These results open the way to combining materials with different dimensionalities to achieve novel nanoscale architectures with improved photovoltaic and light emitting functionalities.
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    HIF-1α-PDK1 Axis-Induced Active Glycolysis Plays an Essential Role in Macrophage Migratory Capacity
    (American Physical Society) Anand, Benoy; Sampat, Siddharth; Danilov, E. O.; Peng, Weina; Rupich, Sara M.; Chabal, Yves J.; Gartstein, Yuri N.; Malko, Anton V.; 0000 0001 1969 6683 (Gartstein, YN); 0000 0001 2678 9765 (Malko, AV); 170647442 (Gartstein, YN); Anand, Benoy; Sampat, Siddharth; Peng, Weina; Rupich, Sara M.; Chabal, Yves J.; Gartstein, Yuri N.; Malko, Anton V.
    Ultrafast transient pump-probe measurements of thin CH₃NH₃PbI₃ perovskite films over a wide spectral range from 350 to 800 nm reveal a family of photoinduced bleach (PB) and absorption (PA) features unequivocally pointing to the fundamentally multiband character of the underlying electronic structure. Excitation pump-energy dependent kinetics of three long-lived PB peaks at 1.65, 2.55, and 3.15 eV along with a broad PA band shows the involvement of band-edge thermalized carriers in all transitions and at least four, possibly more, electronic bands. The evolution of the transient signatures is described in terms of the redistribution of the conserved oscillator strength of the whole system. The multiband perspective opens up different directions for understanding and controlling photoexcitations in hybrid perovskites.
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    Influence of Growth Temperature on Bulk and Surface Defects in Hybrid Lead Halide Perovskite Films
    (Royal Society of Chemistry, 2015-12-14) Peng, Weina; Anand, Benoy; Liu, Lihong; Sampat, Siddharth; Bearden, Brandon E.; Malko, Anton V.; Chabal, Yves J.
    The rapid development of perovskite solar cells has focused its attention on defects in perovskites, which are gradually realized to strongly control the device performance. A fundamental understanding is therefore needed for further improvement in this field. Recent efforts have mainly focused on minimizing the surface defects and grain boundaries in thin films. Using time-resolved photoluminescence spectroscopy, we show that bulk defects in perovskite samples prepared using vapor assisted solution process (VASP) play a key role in addition to surface and grain boundary defects. The defect state density of samples prepared at 150 °C (~10¹⁷ cm⁻³) increases by 5 fold at 175 °C even though the average grains size increases slightly, ruling out grain boundary defects as the main mechanism for the observed differences in PL properties upon annealing. Upon surface passivation using water molecules, the PL intensity and lifetime of samples prepared at 200 °C are only partially improved, remaining significantly lower than those prepared at 150 °C. Thus, the present study indicates that the majority of these defect states observed at elevated growth temperatures originates from bulk defects and underscores the importance to control the formation of bulk defects together with grain boundary and surface defects to further improve the optoelectronic properties of perovskites.
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    Chemical Bonding and Defect States of LPCVD Grown Silicon-Rich Si₃N₄ for Quantum Dot Applications
    (A V S: Science & Technology of Materials, Interfaces, and Processing, 2014-03) Mohammed, Shakil; Nimmo, Michael T.; Malko, Anton V.; Hinkle, Christopher L.; 0000 0001 2678 9765 (Malko, AV); Mohammed, Shakil; Nimmo, Michael T.; Malko, Anton V.; Hinkle, Christopher L.
    Si-rich Si₃N₄ (SRN) thin films were investigated to understand the various defect states present within the SRN that can lead to reduced performance in quantum dot based devices made of these materials. The SRN films, deposited by low pressure chemical vapor deposition followed by furnace anneals over a range of temperatures, were determined to be comprised of two distinct phase separated SRN regions with different compositions (precipitates within a host matrix). Photoluminescence (PL) spectra showed multiple peaks convoluted together within the visible and near-visible range. Depending on deposition and annealing conditions, the films displayed changes in PL peak intensities which were correlated with chemical bonding utilizing x-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, spectroscopic ellipsometry, and capacitance-voltage measurements. It is found that the PL originates from defect-state to defect-state and band edge to defect-state electronic transitions.
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    Energy Transfer from Colloidal Nanocrystals into Si Substrates Studied via Photoluminescence Photon Counts and Decay Kinetics
    (2013-08-16) Nguyen, H. M.; Seitz, Oliver; Gartstein, Yuri N.; Chabal, Yves J.; Malko, Anton V.; 0000 0001 2678 9765 (Malko, AV); Nguyen, H. M.; Seitz, Oliver; Gartstein, Yuri N.; Chabal, Yves J.; Malko, Anton V.
    We use time-resolved photoluminescence (PL) kinetics and PL intensity measurements to study the decay of photoexcitations in colloidal CdSe/ZnS nanocrystals grafted on SiO₂ - Si substrates with a wide range of the SiO₂ spacer layer thicknesses. The salient features of experimental observations are found to be in good agreement with theoretical expectations within the framework of modification of spontaneous decay of electric-dipole excitons by their environment. Analysis of the experimental data reveals that energy transfer (ET) from nanocrystals into Si is a major enabler of substantial variations in decay rates, where we quantitatively distinguish contributions from nonradiative and radiative ET channels. We demonstrate that time-resolved PL kinetics provides a more direct assessment of ET, while PL intensity measurements are also affected by the specifics of the generation and emission processes.
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    Influence of the Core Size on Biexciton Quantum Yield of Giant CdSe/CdS Nanocrystals
    (The Royal Society of Chemistry, 2014-02-06) Mangum, B. D.; Sampat, Siddharth; Ghosh, Y.; Hollingsworth, J. A.; Htoon, H.; Malko, Anton V.; 0000 0001 2678 9765 (Malko, AV); Sampat, Siddharth; Malko, Anton V.
    We present a systematic study of photoluminescence (PL) emission intensity and biexciton (BX) quantum yields (QY_{BX}) in individual "giant" CdSe/CdS nanocrystals (g-NCs) as a function of g-NC core size and shell thickness. We show that g-NC core size significantly affects QY_{BX} and can be utilized as an effective tuning parameter towards higher QY_{BX} while keeping the total volume of the g-NC constant. Specifically, we observe that small-core (2.2 nm diameter) CdSe/CdS NCs with a volume of ~200 nm³ (shell comprises 4 CdS monolayers) show very low average and maximum QY_{BX}'s of ~3 and 7%, respectively. In contrast, same-volume medium-core (3 nm diameter) NCs afford higher average values of ~10%, while QY_{BX}'s of ~30% are achieved for same-volume large-core (5.5 nm diameter) CdSe/CdS NCs, with some approaching ~80%. These observations underline the influence of the g-NC core size on the evolution of PL emissive states in multi-shell NCs. Moreover, our study also reveals that the use of long anneal times in the growth of CdS shells plays a critical role in achieving high QY_{BX}.

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