Time-domain observation of interlayer exciton formation and thermalization in a MoSe2/WSe2 heterostructure

Additional details of experimental conditions for all data herein are presented in the associated manuscript. // LinearAbsorption_MoSe2WSe2-77k.txt for Figure 1b 77K linear absorption spectrum of MoSe2/WSe2 HS. The first column is photon energy with the spectrum the second column. PL_MoSe2WSe2-77k.txt for Figure 1b 77K Photoluminescence spectrum of MoSe2/WSe2 HS. The first column is photon energy with the spectrum the second column. // TA_HighRepRate_MoSe2WSe2-4deg-77k-CCP.txt for Figure 2c Transient absorption measurement of a 4° twist angle MoSe2/WSe2 TMD HS; measurements are performed on a high repetition rate, monochromatically-resolved instrument at 77K and with co-circularly polarized pump and probe. The pump is tuned to 1.58 eV. Data is preprocessed in the following way: differential spectrum are calculated; the data is chirp corrected by fitting the rise to a polynomial; pump scatter is subtracted using spectrum before time zero. Data presented in matrix format: time delay across rows in units of femtoseconds photon energy across columns in units of eletronvolts Transient absorption difference spectra (T_pumpon - T_pumpoff)/T_pumpoff) // TA_SpectrallyResolved_MoSe2WSe2-4deg-77k-CCP.txt for Figure 2a&b Transient absorption measurement of a 4° twist angle MoSe2/WSe2 TMD HS; measurements are performed on a spectrally-resolved instrument at 77K and with co-circularly polarized pump and probe. The pump is tuned to 1.58 eV. Data is preprocessed in the following way: differential spectrum are calculated; the data is chirp corrected by fitting the rise to a polynomial; pump scatter is subtracted using spectrum before time zero. Data presented in matrix format: time delay across columns in units of femtoseconds photon energy across rows in units of eletronvolts Transient absorption difference spectra (T_pumpon - T_pumpoff)/T_pumpoff) // Data for Figure 3e-h: Pulses.dat; Delta_T_hetero_W.dat; Delta_T_hetero_M.dat; Delta_T_hetero_aligned_IL.dat Calculated DTS signatures for the optical response of the A_W (..._W), A_Mo (..._M), and ILX (..._IL) states. The first column in each file corresponds to the pump probe time delay; the columns that follow are the data of the traces organized according to the key in Figure 3e-h. Pulse.dat shows the optical pulse where the first column is the time and the second column is the pulse envelope. // Data for Figure 4b: DWfile.dat; DILfile.dat; ksnapshots_77K_h2_e1_TT_1s.dat, where TT = [400, 800, 2000, 8000, 20000]. Calculated Pauli Blocking weights (DWfile & DILfile) for the A_W and ILX, respectively. The first column corresponds to the COM and the second to the weighting factors. Calculated momentum-dependent excitonic populations of the ILX (ksnapshot...) for pump probe delays of 400, 800, 2000, 8000, and 20000 fs. The first column corresponds to the COM and the second to the excitonic populations