Control of gain and nonlinearities in extremely anisotropic confined semiconductors

• Applicant: Dr. Alexander Achtstein
• Subject Area: Experimental Condensed Matter Physics
• Term: from 2016 to 2023
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 324765876

• Final Report Year: 2023

Final Report Abstract

In the first project period we demonstrated directed emission from CdSe nanoplatelets (NPLs) and investigated the microscopic origin, also for two-photon absorption. We showed that exciton-phonon interaction and strain can be tuned by particle size and coating with ligands or different semiconductor material, causing considerable shifts of emission energy. Using an external electric field we determined the exciton binding energy in CdSe NPLs and found a dipole moment polarizability in the PL dynamics. The second period investigated the scaling of exciton and trion radiative rates and binding energies with 2D nanoparticle size as well as the exciton relative motion mobility on them. In a last, broad section the applicant has studied the frequency-dependent properties of electrons, holes, excitons and trions on different 1D and 2D semiconductor nanoparticles. It is shown that dephasing and thermal population are key quantities to be taken into account in the analysis of experimental THz transport data. Kubo theory however, lacks an additional mobility contribution, which in a master equations based theory is identified as the equilibration current, suppressing e.g. the low-frequency mobility of charges on an 1D domain, a fully new, quantum mechanical phenomenon.

Publications

• Time-Resolved Stark Spectroscopy in CdSe Nanoplatelets: Exciton Binding Energy, Polarizability, and Field-Dependent Radiative Rates. Nano Letters, 16(10), 6576-6583.
  Scott, Riccardo; Achtstein, Alexander W.; Prudnikau, Anatol V.; Antanovich, Artsiom; Siebbeles, Laurens D. A.; Artemyev, Mikhail & Woggon, Ulrike
  
• A strain-induced exciton transition energy shift in CdSe nanoplatelets: the impact of an organic ligand shell. Nanoscale, 9(45), 18042-18053.
  Antanovich, A.; Achtstein, A. W.; Matsukovich, A.; Prudnikau, A.; Bhaskar, P.; Gurin, V.; Molinari, M. & Artemyev, M.
  
• Directed emission of CdSe nanoplatelets originating from strongly anisotropic 2D electronic structure. Nature Nanotechnology, 12(12), 1155-1160.
  Scott, Riccardo; Heckmann, Jan; Prudnikau, Anatol V.; Antanovich, Artsiom; Mikhailov, Aleksandr; Owschimikow, Nina; Artemyev, Mikhail; Climente, Juan I.; Woggon, Ulrike; Grosse, Nicolai B. & Achtstein, Alexander W.
  
• Directed Two-Photon Absorption in CdSe Nanoplatelets Revealed byk-Space Spectroscopy. Nano Letters, 17(10), 6321-6329.
  Heckmann, Jan; Scott, Riccardo; Prudnikau, Anatol V.; Antanovich, Artsiom; Owschimikow, Nina; Artemyev, Mikhail; Climente, Juan I.; Woggon, Ulrike; Grosse, Nicolai B. & Achtstein, Alexander W.
  
• Mobility and Decay Dynamics of Charge Carriers in One-Dimensional Selenium van der Waals Solid. The Journal of Physical Chemistry C, 121(34), 18917-18921.
  Bhaskar, Prashant; Achtstein, Alexander W.; Diedenhofen, Silke L. & Siebbeles, Laurens D. A.
  
• Sideband pump-probe technique resolves nonlinear modulation response of PbS/CdS quantum dots on a silicon nitride waveguide. APL Photonics, 3(1).
  Kolarczik, Mirco; Ulbrich, Christian; Geiregat, Pieter; Zhu, Yunpeng; Sagar, Laxmi Kishore; Singh, Akshay; Herzog, Bastian; Achtstein, Alexander W.; Li, Xiaoqin; van Thourhout, Dries; Hens, Zeger; Owschimikow, Nina & Woggon, Ulrike
  
• Biexciton fine structure in monolayer transition metal dichalcogenides. Nature Physics, 14(12), 1199-1204.
  Steinhoff, Alexander; Florian, Matthias; Singh, Akshay; Tran, Kha; Kolarczik, Mirco; Helmrich, Sophia; Achtstein, Alexander W.; Woggon, Ulrike; Owschimikow, Nina; Jahnke, Frank & Li, Xiaoqin
  
• Charge Mobility and Recombination Mechanisms in Tellurium van der Waals Solid. The Journal of Physical Chemistry C, 123(1), 841-847.
  Bhaskar, Prashant; Achtstein, Alexander W.; Vermeulen, Martien J. W. & Siebbeles, Laurens D. A.
  
• Exciton–phonon coupling in mono- and bilayer MoTe 2. 2D Materials, 5(4), 045007.
  Helmrich, Sophia; Schneider, Robert; Achtstein, Alexander W.; Arora, Ashish; Herzog, Bastian; de Vasconcellos, Steffen Michaelis; Kolarczik, Mirco; Schöps, Oliver; Bratschitsch, Rudolf; Woggon, Ulrike & Owschimikow, Nina
  
• Impact of Shell Growth on Recombination Dynamics and Exciton–Phonon Interaction in CdSe–CdS Core–Shell Nanoplatelets. ACS Nano, 12(9), 9476-9483.
  Achtstein, Alexander W.; Marquardt, Oliver; Scott, Riccardo; Ibrahim, Mohamed; Riedl, Thomas; Prudnikau, Anatol V.; Antanovich, Artsiom; Owschimikow, Nina; Lindner, Jörg K. N.; Artemyev, Mikhail & Woggon, Ulrike
  
• Tuning Intraband and Interband Transition Rates via Excitonic Correlation in Low-Dimensional Semiconductors. ACS Photonics, 5(9), 3680-3688.
  Planelles, Josep; Achtstein, Alexander W.; Scott, Riccardo; Owschimikow, Nina; Woggon, Ulrike & Climente, Juan I.
  
• A comparative study demonstrates strong size tunability of carrier–phonon coupling in CdSe-based 2D and 0D nanocrystals. Nanoscale, 11(9), 3958-3967.
  Scott, Riccardo; Prudnikau, Anatol V.; Antanovich, Artsiom; Christodoulou, Sotirios; Riedl, Thomas; Bertrand, Guillaume H. V.; Owschimikow, Nina; Lindner, Jörg K. N.; Hens, Zeger; Moreels, Iwan; Artemyev, Mikhail; Woggon, Ulrike & Achtstein, Alexander W.
  
• Broadband Semiconductor Light Sources Operating at 1060 nm Based on InAs:Sb/GaAs Submonolayer Quantum Dots. IEEE Journal of Selected Topics in Quantum Electronics, 25(6), 1-10.
  Herzog, Bastian; Lingnau, Benjamin; Kolarczik, Mirco; Helmrich, Sophia; Achtstein, Alexander W.; Thommes, Kevin; Alhussein, Fuad; Quandt, David; Strittmatter, Andre; Pohl, Udo W.; Brox, Olaf; Weyers, Markus; Woggon, Ulrike; Ludge, Kathy & Owschimikow, Nina
  
• Size-dependent exciton substructure in CdSe nanoplatelets and its relation to photoluminescence dynamics. Nanoscale, 11(25), 12230-12241.
  Specht, Judith F.; Scott, Riccardo; Corona, Castro Marta; Christodoulou, Sotirios; Bertrand, Guillaume H. V.; Prudnikau, Anatol V.; Antanovich, Artsiom; Siebbeles, Laurens D. A.; Owschimikow, Nina; Moreels, Iwan; Artemyev, Mikhail; Woggon, Ulrike; Achtstein, Alexander W. & Richter, Marten
  
• Two-photon based pulse autocorrelation with CdSe nanoplatelets. Nanoscale, 11(37), 17293-17300.
  Quick, Michael T.; Owschimikow, Nina; Khan, Ali Hossain; Polovitsyn, Anatolii; Moreels, Iwan; Woggon, Ulrike & Achtstein, Alexander W.
  
• Unconventional Thermally Activated Indirect to Direct Radiative Recombination of Electrons and Holes in Tin Disulfide Two-Dimensional van der Waals Material. The Journal of Physical Chemistry C, 123(18), 11968-11973.
  Bhaskar, Prashant; Achtstein, Alexander W.; Vermeulen, Martien J. W. & Siebbeles, Laurens D. A.
  
• Tuning trion binding energy and oscillator strength in a laterally finite 2D system: CdSe nanoplatelets as a model system for trion properties. Nanoscale, 12(27), 14448-14458.
  Ayari, Sabrine; Quick, Michael T.; Owschimikow, Nina; Christodoulou, Sotirios; Bertrand, Guillaume H. V.; Artemyev, Mikhail; Moreels, Iwan; Woggon, Ulrike; Jaziri, Sihem & Achtstein, Alexander W.
  
• Electrophoretically-Deposited CdSe Quantum Dot Films for Electrochromic Displays and Smart Windows. ACS Applied Nano Materials, 4(7), 6974-6984.
  Aniskevich, Yauhen; Radchanka, Aliaksandra; Antanovich, Artsiom; Prudnikau, Anatol; Quick, Michael T.; Achtstein, Alexander W.; Jo, Jae Hyeon; Ragoisha, Genady; Artemyev, Mikhail & Streltsov, Eugene
  
• High phonon-limited mobility of charged and neutral excitons in mono- and bilayerMoTe2. 2D Materials.
  Helmrich, Sophia; Achtstein, Alexander W.; Ahmad, Hery; Kunz, Matthias; Herzog, Bastian; Schoeps, Oliver; Woggon, Ulrike & Owschimikow, Nina
  
• Phonon-Assisted Intervalley Scattering Determines Ultrafast Exciton Dynamics in MoSe2 Bilayers. Physical Review Letters, 127(15).
  Helmrich, Sophia; Sampson, Kevin; Huang, Di; Selig, Malte; Hao, Kai; Tran, Kha; Achstein, Alexander; Young, Carter; Knorr, Andreas; Malic, Ermin; Woggon, Ulrike; Owschimikow, Nina & Li, Xiaoqin
  
• Terahertz Charge Carrier Mobility in 1D and 2D Semiconductor Nanoparticles. The Journal of Physical Chemistry Letters, 12(32), 7688-7695.
  Quick, Michael T.; Owschimikow, Nina & Achtstein, Alexander W.
  
• Population dependence of THz charge carrier mobility and non-Drude-like behavior in short semiconductor nanowires. Nanoscale, 14(1), 19-25.
  Achtstein, Alexander W.; Owschimikow, Nina & Quick, Michael T.
  
• Quantum Nature of THz Conductivity: Excitons, Charges, and Trions in 2D Semiconductor Nanoplatelets and Implications for THz Imaging and Solar Hydrogen Generation. ACS Applied Nano Materials, 5(6), 8306-8313.
  Quick, Michael T.; Ayari, Sabrine; Owschimikow, Nina; Jaziri, Sihem & Achtstein, Alexander W.
  
• THz Response of Charge Carriers in Nanoparticles: Microscopic Master Equations Reveal an Unexplored Equilibration Current and Nonlinear Mobility Regimes. Advanced Photonics Research, 4(2).
  Quick, Michael T.; Wach, Quentin; Owschimikow, Nina & Achtstein, Alexander W.
  
• THz mobility and polarizability: impact of transformation and dephasing on the spectral response of excitons in a 2D semiconductor. Physical Chemistry Chemical Physics, 25(4), 3354-3360.
  Quick, Michael T.; Ayari, Sabrine; Owschimikow, Nina; Jaziri, Sihem & Achtstein, Alexander W.