
1.Research School of Electrical, Energy and Materials Engineering, College of Engineering and Computer Science, The Australian National University, Canberra, ACT 2601, Australia
2.Optical Sciences Centre, Swinburne University of Technology, Hawthorn, VIC 3122, Australia
3.ARC Centre of Excellence for Future Low-Energy Electronics Technology, Australia
4.Centre for Quantum Computation and Communication Technology, Department of Quantum Science, Research School of Physics and Engineering, The Australian National University, Acton, ACT 2601, Australia
5.School of Mechatronical Engineering, Beijing Institute of Technology, Beijing 100081, China
6.Institute for Biomedical Materials and Devices (IBMD), Faculty of Science, University of Technology Sydney, Sydney, NSW 2007, Australia
Yuerui Lu (yuerui.lu@anu.edu.au)
Published:2020,
Published Online:06 July 2020,
Received:08 March 2020,
Revised:14 May 2020,
Accepted:09 June 2020
Scan QR Code
Sharma, A. et al. Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit. Light: Science & Applications, 9, 1130-1142 (2020).
Sharma, A. et al. Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit. Light: Science & Applications, 9, 1130-1142 (2020). DOI: 10.1038/s41377-020-00347-y.
Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications. However
most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities
as there are large inhomogeneous broadening and dephasing effects on the transport of excitons in their native states in materials. Here
by confining coherent excitons at the 2D quantum limit
we first observed molecular aggregation-enabled 'supertransport' of excitons in atomically thin two-dimensional (2D) organic semiconductors between coherent states
with a measured high effective exciton diffusion coefficient of ~346.9 cm
2
/s at room temperature. This value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic materials. Without coupling to any optical cavities
the monolayer pentacene sample
a very clean 2D quantum system (~1.2 nm thick) with high crystallinity (J-type aggregation) and minimal interfacial states
showed superradiant emission from Frenkel excitons
which was experimentally confirmed by the temperature-dependent photoluminescence (PL) emi
ssion
highly enhanced radiative decay rate
significantly narrowed PL peak width and strongly directional in-plane emission. The coherence in monolayer pentacene samples was observed to be delocalised over ~135 molecules
which is significantly larger than the values (a few molecules) observed for other organic thin films. In addition
the supertransport of excitons in monolayer pentacene samples showed highly anisotropic behaviour. Our results pave the way for the development of future high-speed excitonic circuits
fast OLEDs
and other optoelectronic devices.
Shen, J. T.&Fan, S. H. Coherent photon transport from spontaneous emission in one-dimensional waveguides.Opt. Lett.30, 2001–2003 (2005)..
Bradac, C. et al. Room-temperature spontaneous superradiance from single diamond nanocrystals.Nat. Commun.8, 1205 (2017)..
Boulais, É. et al. Programmed coherent coupling in a synthetic DNA-based excitonic circuit.Nat. Mater.17, 159–166 (2018)..
Goban, A. et al. Superradiance for atoms trapped along a photonic crystal waveguide.Phys. Rev. Lett.115, 063601 (2015)..
Goldberg, D. et al. Exciton-lattice polaritons in multiple-quantum-well-based photonic crystals.Nat. Photon.3, 662–666 (2009)..
Lopez-Sanchez, O. et al. Ultrasensitive photodetectors based on monolayer MoS2.Nat. Nanotechnol.8, 497–501 (2013)..
Scheibner, M. et al. Superradiance of quantum dots.Nat. Phys.3, 106–110 (2007)..
Reimann, R. et al. Cavity-modified collective rayleigh scattering of two atoms.Phys. Rev. Lett.114, 023601 (2015)..
Chou, C. W. et al. Single-photon generation from stored excitation in an atomic ensemble.Phys. Rev. Lett.92, 213601 (2004)..
Wolke, M. et al. Cavity cooling below the recoil limit.Science337, 75–78 (2012)..
Bohnet, J. G. et al. A steady-state superradiant laser with less than one intracavity photon.Nature484, 78–81 (2012)..
Lunt, R. R. et al. Exciton diffusion lengths of organic semiconductor thin films measured by spectrally resolved photoluminescence quenching.J. Appl. Phys.105, 053711 (2009)..
Imamog-lu, A. et al. Quantum information processing using quantum dot spins and cavity QED.Phys. Rev. Lett.83, 4204–4207 (1999)..
Biolatti, E. et al. Quantum information processing with semiconductor macroatoms.Phys. Rev. Lett.85, 5647–5650 (2000)..
Solinas, P. et al. Holonomic quantum gates: a semiconductor-based implementation.Phys. Rev. A67, 062315 (2003)..
Singh-Rachford, T. N.&Castellano, F. N. Photon upconversion based on sensitized triplet–triplet annihilation.Coord. Chem. Rev.254, 2560–2573 (2010)..
Dicke, R. H. Coherence in spontaneous radiation processes.Phys. Rev.93, 99–110 (1954)..
Abasto, D. F. et al. Exciton diffusion length in complex quantum systems: the effects of disorder and environmental fluctuations on symmetry-enhanced supertransfer.Philos. Trans. R. Soc. A370, 3750–3770 (2012)..
Wan, Y. et al. Direct imaging of exciton transport in tubular porphyrin aggregates by ultrafast microscopy.J. Am. Chem. Soc.139, 7287–7293 (2017)..
Caram, J. R. et al. Room-temperature micron-scale exciton migration in a stabilized emissive molecular aggregate.Nano Lett.16, 6808–6815 (2016)..
Clark, K. A., Krueger, E. L.&Vanden Bout, D. A. Direct measurement of energy migration in supramolecular carbocyanine dye nanotubes.J. Phys. Chem. Lett.5, 2274–2282 (2014)..
Haedler, A. T. et al. Long-range energy transport in single supramolecular nanofibres at room temperature.Nature523, 196–199 (2015)..
Shaw, P. E., Ruseckas, A.&Samuel, I. D. W. Exciton diffusion measurements in poly (3‐hexylthiophene).Adv. Mater.20, 3516–3520 (2008)..
Zhu, T. et al. Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures.Sci. Adv.4, eaao3104 (2018)..
Vörös, Z. et al. Long-distance diffusion of excitons in double quantum well structures.Phys. Rev. Lett.94, 226401 (2005)..
Sun, D. Z. et al. Observation of rapid exciton–exciton annihilation in monolayer molybdenum disulfide.Nano Lett.14, 5625–5629 (2014)..
Wu, S. D., Cheng, L. W.&Wang, Q. Excitonic effects and related properties in semiconductor nanostructures: roles of size and dimensionality.Mater. Res. Express4, 085017 (2017)..
Lunt, R. R., Benziger, J. B.&Forrest, S. R. Relationship between crystalline order and exciton diffusion length in molecular organic semiconductors.Adv. Mater.22, 1233–1236 (2010)..
High, A. A. et al.Control of exciton fluxes in an excitonic integrated circuit.Science321, 229–231 (2008)..
Grosso, G. et al. Excitonic switches operating at around 100 K.Nat. Photon.3, 577–580 (2009)..
Baldo, M.&Stojanović, V. Optical switching: excitonic interconnects.Nat. Photon.3, 558–560 (2009)..
Wan, Y. et al. Cooperative singlet and triplet exciton transport in tetracene crystals visualized by ultrafast microscopy.Nat. Chem.7, 785–792 (2015)..
Lim, S. H. et al. Exciton delocalization and superradiance in tetracene thin films and nanoaggregates.Phys. Rev. Lett.92, 107402 (2004)..
Zhang, Y. H. et al. Probing carrier transport and structure-property relationship of highly ordered organic semiconductors at the two-dimensional limit.Phys. Rev. Lett.116, 016602 (2016)..
Bardeen, C. J. Excitonic processes in molecular crystalline materials.MRS Bull.38, 65–71 (2013)..
Spano, F. C.&Yamagata, H. Vibronic coupling in J-aggregates and beyond: a direct means of determining the exciton coherence length from the photoluminescence spectrum.J. Phys. Chem. B115, 5133–5143 (2011)..
Spano, F. C. The spectral signatures of frenkel polarons in H- and J-aggregates.Acc. Chem. Res.43, 429–439 (2010)..
Würthner, F., Kaiser, T. E.&Saha-Möller, C. R. J-aggregates: from serendipitous discovery to supramolecular engineering of functional dye materials.Angew. Chem. Int. Ed.50, 3376–3410 (2011)..
Cong, K. K. et al. Dicke superradiance in solids.J. Opt. Soc. Am. B33, C80–C101 (2016)..
Marciniak, H. et al. Ultrafast singlet and triplet dynamics in microcrystalline pentacene films.Phys. Rev. B79, 235318 (2009)..
Montali, A. et al. Polarizing energy transfer in photoluminescent materials for display applications.Nature392, 261–264 (1998)..
Hestand, N. J. et al. Polarized absorption in crystalline pentacene: theory vs experiment.J. Phys. Chem. C119, 22137–22147 (2015)..
Kato, T.&Kaneko, T. Transport dynamics of neutral excitons and trions in monolayer WS2.ACS Nano10, 9687–9694 (2016)..
Tokar, V. I. Non-Gaussian diffusion profiles caused by mobile impurity-vacancy pairs in the five frequency model of diffusion.arXiv1801, 05285 (2018)..
Ma, X. D. et al. Influences of exciton diffusion and exciton-exciton annihilation on photon emission statistics of carbon nanotubes.Phys. Rev. Lett.115, 017401 (2015)..
Mouri, S. et al. Nonlinear photoluminescence in atomically thin layered WSe2 arising from diffusion-assisted exciton-exciton annihilation.Phys. Rev. B90, 155449 (2014)..
Akselrod, G. M. et al. Visualization of exciton transport in ordered and disordered molecular solids.Nat. Commun.5, 3646 (2014)..
Jailaubekov, A. E. et al. Hot charge-transfer excitons set the time limit for charge separation at donor/acceptor interfaces in organic photovoltaics.Nat. Mater.12, 66–73 (2013)..
Saikin, S. K. et al. Photonics meets excitonics: natural and artificial molecular aggregates.Nanophotonics2, 21–38 (2013)..
Lloyd, S.&Mohseni, M. Symmetry-enhanced supertransfer of delocalized quantum states.New J. Phys.12, 075020 (2010)..
Chuang, C. et al. Quantum diffusion on molecular tubes: Universal scaling of the 1D to 2D transition.Phys. Rev. Lett.116, 196803 (2016)..
Rao, A. et al. Exciton fission and charge generation via triplet excitons in pentacene/C60 bilayers.J. Am. Chem. Soc.132, 12698–12703 (2010)..
Smith, M. B.&Michl, J. Singlet fission.Chem. Rev.110, 6891–6936 (2010)..
Piland, G. B. et al. Singlet fission: from coherences to kinetics.J. Phys. Chem. Lett.5, 2312–2319 (2014)..
Jundt, C. et al. Exciton dynamics in pentacene thin films studied by pump-probe spectroscopy.Chem. Phys. Lett.241, 84–88 (1995)..
Wilson, M. W. B. et al. Singlet exciton fission in polycrystalline pentacene: from photophysics toward devices.Acc. Chem. Res.46, 1330–1338 (2013)..
Lukman, S. et al. Tuning the role of charge-transfer states in intramolecular singlet exciton fission through side-group engineering.Nat. Commun.7, 13622 (2016)..
Lukman, S. et al. Tuneable singlet exciton fission and triplet–triplet annihilation in an orthogonal pentacene dimer.Adv. Funct. Mater.25, 5452–5461 (2015)..
Roberts, S. T. et al. Efficient singlet fission discovered in a disordered acene film.J. Am. Chem. Soc.134, 6388–6400 (2012)..
Yost, S. R. et al. A transferable model for singlet-fission kinetics.Nat. Chem.6, 492–497 (2014)..
Burgess, T. et al. Doping-enhanced radiative efficiency enables lasing in unpassivated GaAs nanowires.Nat. Commun.7, 11927 (2016)..
Bergmann, L. et al. Direct observation of intersystem crossing in a thermally activated delayed fluorescence copper complex in the solid state.Sci. Adv.2, e1500889 (2016)..
0
Views
0
Downloads
0
CSCD
Publicity Resources
Related Articles
Related Author
Related Institution
京公网安备11010802024621