EFFECTIVE MASS AND MOMENTUM RESOLVED INTRINSIC LINEWIDTH OF IMAGE-POTENTIAL STATES ON Ag(100) Claudio Giannetti INFM and Università Cattolica del Sacro Cuore Dipartimento di Matematica e Fisica, Via Musei 41 Brescia. INFM DMF INFMeeting, Genova 23-25 Giugno 2003 INTRODUCTION •Femtosecond Laser and tunability of photon energy → Non-Linear Photoemission •Study of image-potential states on Ag(100) at different photon energies: effective masses and lifetimes. •WHY IMAGE POTENTIAL STATES? Relaxation of electrons into bulk states can be studied directly in the timedomain with pump-probe techniques. U. Höfer et al., Science 277, 1480 (1997). W. Berthold et al., Phys. Rev. Lett. 88, 056805 (2002). It is a many body interesting problem. A.García-Lekue et al., Phys. Rev. Lett. 89, 096401 (2002). J. Kliewer et al., Science 288, 1399 (2000). Interplay between image-potential states and dynamics of molecules at surfaces. A. D. Miller et al., Science 297, 1163 (2002). INFM DMF INFMeeting, Genova 23-25 Giugno 2003 LASER APPARATUS Ti:Sapphire laser system: Amplified Ti:Sapphire oscillator Tunability: 750-850nm Pulse width: 150fs Rep. rate: 1kHz Average Power: 0.5W Travelling-wave optical parametric generation (TOPG): Tunability: 1150-1500nm (0.8-1.1 eV) 4th (3.2-4.4 eV) Average power 30mW INFM DMF INFMeeting, Genova 23-25 Giugno 2003 ULTRA-HIGH-VACUUM SYSTEM m-metal UHV chamber B<10 mG Base pressure <2x10-10 mbar photoemitted electrons detector: time of flight spectrometer (TOF) TOF: ToF length = 432 mm Temporal resolution = 0.5 ns Acceptance angle = 2.6° Energy resolution about 30 meV @ 2eV PS1 PS2 GPIB Laser start PS3 PS4 PC Preamplifier Discriminator Multiscaler FAST 7887 stop INFM DMF INFMeeting, Genova 23-25 Giugno 2003 IMAGE-POTENTIAL STATES ON METALS Coulomb potential due to electronic image-charge: V(z)1/z forbidden gap in bulk states Image-charge of an electron at a metal surface. 2-D electron gas Ag(100) n=1 n=2 Rydberg series: En U. Hofer, I.L. Shumay, Ch. Reuß, U. Thomann, W. Wallauer, Th. Fauster, Science 277, 1480 (1997). INFM DMF INFMeeting, Genova 23-25 Giugno 2003 0.85eV (n a)2 DISPERSION OF IS Band structure of Ag(100) 2 2 k // E (k // ) En 2m* En: binding energy m*: effective mass INFM DMF INFMeeting, Genova 23-25 Giugno 2003 IS SPECTRA Ebin= 0.5eV 2-photon photoemission Ekin = h-Ebin Ag(100) h=4.32 eV n=1 FWHM: 62meV n=2 FWHM: 52meV Efermi RADIATION: Polarization: P Incident angle: 30° INFM DMF INFMeeting, Genova 23-25 Giugno 2003 SELECTION RULES DIPOLE SELECTION RULES: Ag(100) n S P J=0 J≠0 in S-polarization in P-polarization J is the current density associated to image-potential states INFM DMF INFMeeting, Genova 23-25 Giugno 2003 IS DISPERSION 2-Dimensional electron gas: DISPERSION k|| 2mEKin sin 2 2 k // E (k // ) En 2m* Intensity (log scale) n=1 n=2 Ag(100) Ekin (eV) G.Ferrini, C.Giannetti, D.Fausti, G.Galimberti, M.Peloi, G.P.Banfi, F.Parmigiani, PRB 67, 235407 (2003). INFM DMF INFMeeting, Genova 23-25 Giugno 2003 EFFECTIVE MASS m* d 2 E / dk||2 n=2 n=2 n=1 n=1 Measured values n=1 n=2 0.99±0.02 0.97±0.02 1.15±0.1* 2 1.06±0.09 1.03±0.06 Calculated values n=1 n=2 0.95* 1.03** 1.03** * K.Giesen et al., PRB 35 975 (1987). ** Z.Li and S.Gao , PRB 50 15349 (1994). INFM DMF INFMeeting, Genova 23-25 Giugno 2003 IS LIFETIMES FITTING: Gaussian-Lorentzian convolution Gaussian: experimental resolution FWHM45meV Lorentzian: intrinsic linewidth 14meV @ k//=0 LIFETIME / Measured values (fs) n=1 n=2 47±7 55±5# ≥55 160±10# 658meV fs Calculated values (fs) n=1 n=2 55## 132## # # I.L.Shumay et al., PRB 58 13974 (1998). ## A.García-Lekue et al., Phys. Rev. Lett. 89, 096401 (2002). ### E.V Chulkov et al., Surf. Sci 391 L1217 (1997). Linewidth dependance on k// INFM DMF INFMeeting, Genova 23-25 Giugno 2003 FIRST OBSERVATION OF IMAGE STATES OUT OF RESONANCE e- E EV h3.14eVDE 0.5 eV n=1 e- DE=3.8 eV EF intensity intensity Fermi edge Fermi edge LOG LIN SCALE SCALE Ekin kin (eV) Ekin= h-Ebin= (3.14-0.5)eV 2.7eV INFM DMF INFMeeting, Genova 23-25 Giugno 2003 DISPERSION AND SELECTION RULES Fermi edge n=1 m*/m0.95 Ekin= h-Ebin Dh=0.39eV h=3.15eV h=3.54eV EV Ebin n=1 eEF INFM DMF INFMeeting, Genova 23-25 Giugno 2003 SELECTION RULES Ag(100) n S P DIPOLE SELECTION RULES: J=0 in S-polarization J≠0 in P-polarization WHICH IS THE POPULATION AND PHOTOEMISSION MECHANISM? We can exclude: Role of surface roughness Ponderomotive and tunnel effects at the surface, because the radiation intensity is too low. (I~0.1GW/cm2) INFM DMF INFMeeting, Genova 23-25 Giugno 2003 CONCLUSIONS •Non-linear photoemission on image-potential states in Ag(100). • Improvement of the precision in the measurement of the effective masses and lifetimes. • Observation of image-potential states also when hE1-Efermi. In this case the imagepotential states can be populated and photoemitted also in S-polarization. INFM DMF INFMeeting, Genova 23-25 Giugno 2003 Responsibles: Co-workers: F. Parmigiani, G. Ferrini. F. Banfi, D. Fausti, G. Galimberti, S. Pagliara, M. Peloi. INFM DMF INFMeeting, Genova 23-25 Giugno 2003