Zhang, YeYeZhangLiu, RenhuiRenhuiLiuHuang, JianqiJianqiHuangTUAN HUNG NGUYENSaito, RiichiroRiichiroSaitoYang, TengTengYangZhang, ZhidongZhidongZhang2025-09-242025-09-242025https://www.scopus.com/inward/record.uri?eid=2-s2.0-105002266195&doi=10.1002%2Fjrs.6768&partnerID=40&md5=a78bde0095c41ef892e2652028309e71https://scholars.lib.ntu.edu.tw/handle/123456789/732284We calculate double-resonance Raman (DRR) spectra of monolayer graphene by first-principles density functional calculation, for wide laser excitation energies from the near-infrared (1.58 eV) to the deep-ultraviolet (DUV, 5.41 eV) region. When laser excitation energy, (Formula presented.), goes into the DUV region, Raman peak wavenumber for G (Formula presented.) band switches from red-shift to blue-shift and for 2D (Formula presented.) band switches from red-shift to constant, in contrast to the continuous blue-shift of G (Formula presented.) band. Raman intensity of the three bands generally decreases with increasing (Formula presented.), except for (Formula presented.) around 4.08 eV where Raman intensity diverges due to van Hove singularity of electron density of states. The combined two-phonon modes change with (Formula presented.) for both G (Formula presented.) and G (Formula presented.) bands (e.g., from 2LO to 2TO and back to 2LO for G (Formula presented.) and from LA + LO/TO to TA + LO/TO for G (Formula presented.)) but remain 2LO for 2D (Formula presented.) band. Further, the dominant DRR scattering process of G (Formula presented.) band changes from the electron-hole ((Formula presented.) or (Formula presented.)) scattering processes to the (Formula presented.) scattering processes as (Formula presented.) goes into the DUV region, since the Dirac energy bands become asymmetric between (Formula presented.) and (Formula presented.) band that suppresses the (Formula presented.) process and the Raman intensity. Another factor to suppress the Raman intensity is the quantum interference effect between four scattering processes ((Formula presented.)) which changes from constructive to destructive interference and finally to no interference with increasing (Formula presented.). We calculate (Formula presented.) -dependent Raman tensor of the three bands and polarized Raman spectra, which further support the interference effect. The calculated results are directly compared and consistent with the experimental results.Blue ShiftElectron Density MeasurementElectron ScatteringExcitation EnergyQuantum Interference DevicesRaman ScatteringRed ShiftDeep UltravioletDeep-ultraviolet RegionsDouble ResonanceEnergyGraphenesInterference EffectsRaman IntensitiesRed ShiftScattering ProcessLaser Excitation[SDGs]SDG7journal article10.1002/jrs.67682-s2.0-105002266195