Ultrafast Coherent Exciton Couplings and Many-Body Interactions in Monolayer WS2

被引:10
作者
Timmer, Daniel [1 ]
Gittinger, Moritz [1 ]
Quenzel, Thomas [1 ]
Cadore, Alisson R. [2 ]
Rosa, Barbara L. T. [2 ]
Li, Wenshan [2 ]
Soavi, Giancarlo [2 ,3 ,4 ]
Lunemann, Daniel C. [1 ]
Stephan, Sven [1 ,5 ]
Silies, Martin [1 ,5 ]
Schulz, Tommy [6 ,7 ]
Steinhoff, Alexander [6 ,7 ]
Jahnke, Frank [6 ,7 ]
Cerullo, Giulio [8 ,9 ]
Ferrari, Andrea C. [2 ]
De Sio, Antonietta [1 ,10 ]
Lienau, Christoph [1 ,10 ]
机构
[1] Carl von Ossietzky Univ Oldenburg, Inst Phys, D-26129 Oldenburg, Germany
[2] Univ Cambridge, Cambridge Graphene Ctr, Cambridge CB3 0FA, England
[3] Friedrich Schiller Univ Jena, Inst Solid State Phys, Max Wien Pl 1, D-07743 Jena, Germany
[4] Friedrich Schiller Univ Jena, Abbe Ctr Photon, Albert Einstein Str 6, D-07745 Jena, Germany
[5] Univ Appl Sci, Inst Lasers & Opt, D-26723 Emden, Germany
[6] Univ Bremen, Inst Theoret Phys, D-28334 Bremen, Germany
[7] Univ Bremen, Bremen Ctr Computat Mat Sci, D-28334 Bremen, Germany
[8] Politecn Milan, Dipartimento Fis, I-20133 Milan, Italy
[9] Ist Foton & Nanotecnol IFN CNR, I-20133 Milan, Italy
[10] Carl Von Ossietzky Univ Oldenburg, Ctr Nanoscale Dynam CENAD, Inst Phys, D-26129 Oldenburg, Germany
基金
英国工程与自然科学研究理事会;
关键词
transition metal dichalcogenides; ultrafast spectroscopy; many-body interactions; coherent couplings; MOS2; SPECTROSCOPY; DYNAMICS; GRAPHENE;
D O I
10.1021/acs.nanolett.4c01991
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Transition metal dichalcogenides (TMDs) are quantum confined systems with interesting optoelectronic properties, governed by Coulomb interactions in the monolayer (1L) limit, where strongly bound excitons provide a sensitive probe for many-body interactions. Here, we use two-dimensional electronic spectroscopy (2DES) to investigate many-body interactions and their dynamics in 1L-WS2 at room temperature and with sub-10 fs time resolution. Our data reveal coherent interactions between the strongly detuned A and B exciton states in 1L-WS2. Pronounced ultrafast oscillations of the transient optical response of the B exciton are the signature of a coherent 50 meV coupling and coherent population oscillations between the two exciton states. Supported by microscopic semiconductor Bloch equation simulations, these coherent dynamics are rationalized in terms of Dexter-like interactions. Our work sheds light on the role of coherent exciton couplings and many-body interactions in the ultrafast temporal evolution of spin and valley states in TMDs.
引用
收藏
页码:8117 / 8125
页数:9
相关论文
共 65 条
[1]   Charge-tuneable biexciton complexes in monolayer WSe2 [J].
Barbone, Matteo ;
Montblanch, Alejandro R. -P. ;
Kara, Dhiren M. ;
Palacios-Berraquero, Carmen ;
Cadore, Alisson R. ;
De Fazio, Domenico ;
Pingault, Benjamin ;
Mostaani, Elaheh ;
Li, Han ;
Chen, Bin ;
Watanabe, Kenji ;
Taniguchi, Takashi ;
Tongay, Sefaattin ;
Wang, Gang ;
Ferrari, Andrea C. ;
Atature, Mete .
NATURE COMMUNICATIONS, 2018, 9
[2]   Inverted valley polarization in optically excited transition metal dichalcogenides [J].
Berghauser, Gunnar ;
Bernal-Villamil, Ivan ;
Schmidt, Robert ;
Schneider, Robert ;
Niehues, Iris ;
Erhart, Paul ;
de Vasconcellos, Steffen Michaelis ;
Bratschitsch, Rudolf ;
Knorr, Andreas ;
Malic, Ermin .
NATURE COMMUNICATIONS, 2018, 9
[3]   Exciton broadening and band renormalization due to Dexter-like intervalley coupling [J].
Bernal-Villamil, Ivan ;
Berghauser, Gunnar ;
Selig, Malte ;
Niehues, Iris ;
Schmidt, Robert ;
Schneider, Robert ;
Tonndorf, Philipp ;
Erhart, Paul ;
de Vasconcellos, Steffen Michaelis ;
Bratschitsch, Rudolf ;
Knorr, Andreas ;
Malic, Ermin .
2D MATERIALS, 2018, 5 (02)
[4]   Optical two-dimensional Fourier transform spectroscopy of semiconductors [J].
Borca, CN ;
Zhang, TH ;
Li, XQ ;
Cundiff, ST .
CHEMICAL PHYSICS LETTERS, 2005, 416 (4-6) :311-315
[5]  
Breuer H. P., 2002, THEORY OPEN QUANTUMS
[6]   Phase-locked pulses for two-dimensional spectroscopy by a birefringent delay line [J].
Brida, Daniele ;
Manzoni, Cristian ;
Cerullo, Giulio .
OPTICS LETTERS, 2012, 37 (15) :3027-3029
[7]  
Brongersma ML, 2015, NAT NANOTECHNOL, V10, P25, DOI [10.1038/NNANO.2014.311, 10.1038/nnano.2014.311]
[8]   Monolayer WS2 electro- and photo-luminescence enhancement by TFSI treatment [J].
Cadore, A. R. ;
Rosa, B. L. T. ;
Paradisanos, I ;
Mignuzzi, S. ;
De Fazio, D. ;
Alexeev, E. M. ;
Dagkli, A. ;
Muench, J. E. ;
Kakavelakis, G. ;
Shinde, S. M. ;
Yoon, D. ;
Tongay, S. ;
Watanabe, K. ;
Taniguchi, T. ;
Lidorikis, E. ;
Goykhman, I ;
Soavi, G. ;
Ferrari, A. C. .
2D MATERIALS, 2024, 11 (02)
[9]   Population inversion and giant bandgap renormalization in atomically thin WS2 layers [J].
Chernikov, Alexey ;
Ruppert, Claudia ;
Hill, Heather M. ;
Rigosi, Albert F. ;
Heinz, Tony F. .
NATURE PHOTONICS, 2015, 9 (07) :466-U69
[10]   Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2 [J].
Chernikov, Alexey ;
Berkelbach, Timothy C. ;
Hill, Heather M. ;
Rigosi, Albert ;
Li, Yilei ;
Aslan, Ozgur Burak ;
Reichman, David R. ;
Hybertsen, Mark S. ;
Heinz, Tony F. .
PHYSICAL REVIEW LETTERS, 2014, 113 (07)