Dataset supporting Highly Tunable Ground and Excited State Excitonic Dipoles in Multilayer 2H-MoSe2

Dataset for Figures 2-5 for 'Highly Tunable Ground and Excited State Excitonic Dipoles in Multilayer 2H-MoSe2':

FIG. 2: Layer hybridised excitons in 2L 2H-MoSe2. a, VE dependence of the first derivative of the reflectance contrast spectra with respect to photon energy (d(ΔR/R0)/dE) in our 2L 2H-MoSe2 in the spectral range 1.68 - 1.78 eV. b, Calculated energies of the different hybrid IX2L-XA2s exciton states as a function of VE, which we label as hX1, hX2, hX3, and hX4 from low to high energy at VE > 0 V, respectively. The colour of the solid lines denotes the contribution of the different bare exciton states to each hybrid exciton. c, Schematics of the spin, valley, and layer configuration of the exciton states responsible for the exciton hybridisation shown in panel a for negative and positive applied VE (left and right panels, respectively). The exciton hybridisation is attributed to a second-order effective coupling between IX2L and the intralayer A exciton facilitated via the A and B exciton admixture (depicted by the glowing double arrows). d, The energy position of IX2L and XA2s as a function of applied electric field, as obtained from GW+BSE calculations. The labels identify the simplified bare exciton states. e Normalized theoretical oscillator strengths (red vertical line) and absorption spectra (black line) at 0 eV/Å and 0.03 eV/Å focusing on the energy range of IX2L and XA2s. The numerical precision of our calculations is estimated to be of the order of ±5 meV, see computational details in Supplementary Note S4.

FIG. 3: Layer hybridised excitons in 3L MoSe2. a, VE dependence of d(ΔR/R0)/dE in the 3L MoSe2 region of our sample. b, Energies of the different hybrid IX3L-XA1s exciton states as a function of VE, where the colour of the solid lines denotes the contribution of the different bare exciton states to each hybrid exciton. c, Schematics of the spin, valley, and layer configuration of the exciton states responsible for the exciton hybridisation shown in panel a for negative and positive applied VE (left and right panels, respectively). The exciton hybridisation is attributed to direct spin-conserving interlayer hole tunnelling between L1 and L3.

FIG. 4: Magneto-optical properties of layer-hybridised excitons in 2L MoSe2 and 3L MoSe2. a, Zeeman splitting of hX4 at three different applied VE. The blue dots represent the experimental values, while the blue solid lines show linear fits of the experimental data, from which we are able to estimate the effective g-factor of this hybrid exciton at each applied VE. b, VE-driven evolution of the g-factor of the hybrid excitons hX3 (-5 to 0 V, red shaded area) and hX4 (0 to 5 V, blue shaded area) in bilayer MoSe2 (bottom panel). The top panel shows the VE-dependent contributions of each bare exciton state|CIX(X)3,4|2 to the corresponding hybrid excitons. c, Zeeman splitting of IX3L at measured at VE = 0 V.

FIG. 5: Observation of excited states of IX2L and IX3L. a, VE dependence of d2(ΔR/R0)/dE2 in a second location of the 2L 2H-MoSe2 sample in the spectral range 1.67 - 1.83 eV. b, d2(ΔR/R0)/dE2 in another location of the 3L 2H-MoSe2 sample in the spectral range 1.58 - 1.8 eV. c Calculated energies of the different exciton states of 2L 2H-MoSe2 including IX2s,2L with same spin and layer configuration as IX2L. d Calculated energies of the different exciton states in 3L 2H-MoSe2 including IX2s,3L with the same spin and layer configuration as IX3L.