High Resolution Nonlinear Spectroscopy of 2D Excitons in Monolayer MoSe$_{2}$

ORAL

Abstract

Monolayer transition metal dichalcogenides (mTMDs), such as MoSe$_{2}$, have emerged as the first truly 2D semiconductors, exhibiting a wide range of novel electro-optical phenomena which arise from the material's graphene-like honeycomb lattice. The optical response of mTMDs is dominated by strongly bound excitons which are localized in momentum space to two sets of inequivalent valleys ($+$K, -K) at the edge of the Brillouin zone. We report the first high resolution nonlinear spectroscopy measurements on monolayer MoSe$_{2}$. Differential reflection measurements reveal that the degenerate nonlinear optical response agrees with the previously reported photoluminescence and reflectivity measurements, showing a broadened linewidth on order of 5 meV. Non-degenerate spectral holeburning measurements reveal narrow optical resonances approximately 1000 times narrower (order of 2 micro eV), indicating that excitons in mTMDs are dominantly inhomogenously broadened and exhibit an intrinsic lifetime on the order of 1 ns, over an order of magnitude longer than all previously reported lifetimes obtained through time domain techniques. Polarization dependent spectral holeburning measurements probe valley dependent processes such as the intervalley relaxation rates.

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Authors

  • John Schaibley

    University of Washington

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University

  • William H. Dowd

    Oregon State University, University of Washington, University of Hong Kong, University of Tennessee, Oak Ridge National Laboratory, University of British Columbia, Univ of Washington, Univ of Cambridge, Michigan State University, Universit\'e de Caen, Argonne National Laboratory, Texas A\&M University -Commerce, Texas A\&M University, Department of Physics, University of Idaho, Moscow, Idaho 83844, USA, Universidad de Salamanca, E-37008 Salamanca, Spain, Department of Physics, Florida State University, Tallahassee, Florida 32306, USA, University of Cambridge, Institute of Astronomy, University of Cambridge, Canadian Institute for Theoretical Astrophysics, University of Toronto, Seoul National University, Chungnam National University, Department of Physics, Oregon State University, TRIUMF, Roosevelt High School, Department of Physics, University of Washington, Oregon State Department of Chemistry, Oregon State School of Electrical Engineering and Computer Science, Oregon State Department of Physics, University of Idaho, Lawrence Livermore National Laboratory, Idaho National Laboratory, Pacific Northwest National Laboratory, Carnegie Institution of Washington, Department of Chemistry, Oregon State University, School of Electrical Engineering and Computer Science, Oregon State University, Washington State University, Harvard University, Idaho Accelerator Center, Idaho Accelerator Center, Idaho State University, 1500 Alvin Ricken drive, Pocatello, ID 83201, USA, CENPA, University of Washington, Physics Division, ANL, NSCL, Michigan State University, Division, ANL, LPC, CAEN, France, Paul Scherrer Institute, US Geological Survey, 12201 Sunrise Valley Drive, Reston, VA, 20192, USA, University of Calgary Department of Physics and Astronomy, University of Calgary Department of Geoscience, None, University of the Fraser Valley, Univ of California, Berkeley, Simon Fraser University, Los Alamos Natl. Lab., University of Science and Technology of China, Hefei, U of Washington, Georgia Institute of Technology, Washington State Univ, National Institute of Standards and Technology and University of Maryland, American University