Time-resolved 2PPE: Probing adsorbate motion on femtosecond time-scales – what is the role of the laser bandwidth?
Source abstract
Abstract
Recently it has been shown that time-resolved two photon photoemission spectroscopy (TR 2PPE) is capable of probing the atomic motion of an adsorbate after excitation by a femtosecond laser-pulse. In this paper we address the question in how far the bandwidth of the used laser pulse is of importance with respect to the sensitivity of TR 2PPE to the actual nuclear dynamics. In particular, we find that the use of laser pulses of different spectral bandwidth may simplify the interpretation of the measured TR 2PPE autocorrelation traces and help to distinguish between purely electron related contributions and the nuclear dynamics. Our experimental results indicate that for pulses of small bandwidth only the lifetime of the electronic adsorbate excitation at the ground state equilibrium distance is probed. This information can be used as input for the interpretation of autocorrelation traces obtained with large bandwidth pulses, which in addition contain information about the nuclear dynamics of the adsorbate.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Electron and X-Ray Spectroscopy Techniques · Advanced Chemical Physics Studies · Nuclear Physics and Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (22)
Show source-provided references
1. See e.g. J.W. Gadzuk, L.J. Richter, S.A. Buntin, R.R. Cavanagh: Surf. Sci. 235, 317 (1990); J.A. Misewich, T.F. Heinz, D.M. Newns: Phys. Rev. Lett. 68, 3737 (1992); S.M. Harris, S. Holloway, G.R. Darling: J.Chem.Phys. 102, 8235 (1995); J.W. Gadzuk: Surf. Sci. 342, 345 (1995)10.1016/0039-6028(90)90807-K ↗
2. See e.g. R.W. Schoenlein, W.Z. Lin, J.G. Fujimoto, G.L. Eesley: Phys. Rev. Lett. 58, 1680 (1987), U. Höfer, I.L. Shumay, C. Reuss, U. Thomann, W. Wallauer, T. Fauster: Science 277, 1480 (1997); N.H. Ge, C.M. Wong, R.L. Lingle, J.D. McNeill, K.J. Gaffney, C.B. Harris: Science 279, 202 (1998); L. Bartels, G. Meyer, K.-H. Rieder, D. Velic, E. Knoesel, A. Hotzel, M. Wolf, G. Ertl: Phys. Rev. Lett. 80, 2004 (1998)10.1103/PhysRevLett.58.1680 ↗
3. M. Bauer, S. Pawlik, M. Aeschlimann: Phys. Rev. B 55, 10040 (1997)10.1103/PhysRevB.55.10040 ↗
4. S. Ogawa, H. Nagano, H. Petek: Phys. Rev. Lett. 82, 1931 (1999)10.1103/PhysRevLett.82.1931 ↗
5. H. Petek, M.J. Weida, H. Nagano, S. Ogawa: Science 288, 1402 (2000)10.1126/science.288.5470.1402 ↗
6. A.G. Borisov, A.K. Kazansky, J.P. Gauyacq: Surf. Sci. 430, 165 (1999)10.1016/S0039-6028(99)00431-8 ↗
7. A.G. Borisov, J.P. Gauyacq, A.K. Kazansky, E.V. Chulkov, V.M. Silkin, P.M. Echenique: Phys. Rev. Lett. 86, 488 (2001)10.1103/PhysRevLett.86.488 ↗
8. M. Bauer, S. Pawlik, R. Burgermeister, M. Aeschlimann: Surf. Sci. 402–404 , 62 (1998)10.1016/S0039-6028(97)01042-X ↗
9. M. Bauer, S. Pawlik, M. Aeschlimann: Phys. Rev. B 60, 5016 (1999)10.1103/PhysRevB.60.5016 ↗
10. S. Ogawa, H. Nagano, H. Petek: Appl. Phys. B 68, 611 (1999)10.1007/s003400050673 ↗
11. H. Petek, M.J. Weida, H. Nagano, S. Ogawa: Surf. Sci. 451, 22 (2000)10.1016/S0039-6028(00)00004-2 ↗
12. A.G. Borisov, J.P. Gauyacq, E.V. Chulkov, V.M. Silkin, P.M. Echenique: Phys. Rev. B 65, 235434 (2002)10.1103/PhysRevB.65.235434 ↗
13. A.G. Borisov, A.K. Kazansky, J.P. Gauyacq: Phys. Rev. B 64, 201105(R) (2001)10.1103/PhysRevB.64.201105 ↗
14. T. Hertel, E. Knoesel, M. Wolf, G. Ertl: Phys. Rev. Lett 76, 535 (1996)10.1103/PhysRevLett.76.535 ↗
15. W. Shockley: Phys. Rev. 56, 317 (1939)10.1103/PhysRev.56.317 ↗
16. P.O. Gartland, B.J. Slagsvold: Phys. Rev. B 12, 4047 (1975)10.1103/PhysRevB.12.4047 ↗
17. R. Panagio, R. Matzdorf, G. Meister, A. Goldmann: Surf. Sci. 336, 113 (1995)10.1016/0039-6028(95)00509-9 ↗
18. 1 ML corresponds to a closely packed alkali layer at the substrate
19. R. Loudon: The Quantum Theory of Light (Oxford University Press, Oxford 1973)
20. In [9] we reported a lifetime for the Cs-resonance of 15±6 fs as average of two limiting cases for T2: the depopulation time T1 and the line-width of the Cs-resonance as observed in the 2PPE spectrum. The best fit in this reference for the former case corresponding to the assumptions made in the present paper results in a lifetime T1 of 12 fs
21. D. Menzel, R. Gomer: J. Chem. Phys. 41, 3311 (1964)10.1063/1.1725730 ↗
22. This value is estimated from the intensity pulse width of 13 fs given in [4] assuming a transform limited, sech2 temporal shaped pulse