Revisiting the thermal-spike concept in ion-surface interactions

In recent years many groups have advocated a thermal-spike model to explain a variety of experimental results in ion-irradiation of solids, as for example sputtering, mixing, compositional change, structural change, and track formation. The latter include crystal-to-amorphous transitions as well as track formation due to MeV/u particles. In this paper we reconsider the phenomena occurring during ion impact of solids looking at the time scale generally indicated as relevant for thermal-spike effects, namely a picosecond scale as shown by molecular dynamics. Sputtering, mixing, and track formation, however, will be analyzed in more detail. We consider first ion-beam sputtering and reiterate (as is already well-known) that yields which increase with the bulk temperature most often indicate merely the onset of normal vaporization. Indeed, only simulations appear to be capable of giving insight even if the information is sometimes tentative. In mixing, ballistic transport is important but not dominant. It is often argued that the additional transport is provided by thermal spikes but it is noted that such an assumption is normally not required by the experimental results. What is more relevant is a role for residual defects such that the total diffusion flux includes (if the defects are chemically guided) a modified Darken factor, or (if the defects are not chemically guided) simply an increased diffusivity. The time scale (min), distances (well beyond the collision cascade), temperature sensitivity (changes of as little as 75 K are relevant), and correlation with vacancy properties (thence with the solid rather than liquid state) which are relevant to these residual defects are not understandable in terms of thermal spikes. We finally consider track formation. Recent work claiming that track formation in solids, irradiated with heavy ions, may be understood in terms of thermal spikes is reconsidered to show that the thermal-spike model is utilized without considering all the relevant phenomena included in irradiation-induced heating and phase transitions. For example, a comparison of fs-laser pulse irradiation of Si with swift heavy-ion irradiation, shows that melting is possible in the first case since the excited electrons have a low and more or less restricted energy while in the case of swift ion-irradiation, the motion of the excited electrons includes a ballistic component which does not favour the localization of the thermal energy necessary to induce lattice melting. It is concluded that track formation is better understandable in a more general framework of defect-induced processes in solids.

[1]  The Se sensitivity of metals under swift-heavy-ion irradiation: a transient thermal process , 1994 .

[2]  R. Yen,et al.  Time-Resolved Reflectivity Measurements of Femtosecond-Optical-Pulse-Induced Phase Transitions in Silicon , 1983 .

[3]  Tom,et al.  Time-resolved study of laser-induced disorder of Si surfaces. , 1988, Physical review letters.

[4]  W. Johnson,et al.  Effect of thermodynamics on ion mixing , 1987 .

[5]  Hsieh,et al.  Effect of temperature on the dynamics of energetic displacement cascades: A molecular dynamics study. , 1989, Physical review. B, Condensed matter.

[6]  R. Kelly The mechanisms of sputtering part I. , 1984 .

[7]  W. Johnson,et al.  Correlation between cohesive energy and mixing rate in ion mixing of metallic bilayers , 1985 .

[8]  I. Baumvol,et al.  Interdiffusion and reaction in the FeAl bilayer: I: Rutherford backscattering analysis of furnace-annealed samples , 1987 .

[9]  F. D. Boer Cohesion in Metals: Transition Metal Alloys , 1989 .

[10]  K. Lieb,et al.  Ion-beam-induced atomic transport and phase formation in the system nickel/antimony , 1993 .

[11]  T. Mitchell,et al.  Electron irradiation damage in quartz , 1974 .

[12]  K. Lieb,et al.  Ion beam mixing and sputtering of Kr-irradiated TiN films measured with RBS, RNRA, and PIXE , 1990 .

[13]  A. Miotello,et al.  Thermodynamic effects in the ion‐beam mixing of Fe‐Al and Mo‐Cr multilayers , 1996 .

[14]  R. Yen,et al.  Picosecond laser‐induced melting and resolidification morphology on Si , 1979 .

[15]  M. Hervieu,et al.  Swift, Heavy Ions in Insulating and Conducting Oxides: Tracks and Physical Properties , 1994 .

[16]  R. Benedek,et al.  Molecular dynamics simulation of displacement cascades in Cu and Ni: Thermal spike behavior , 1989 .

[17]  Fine,et al.  Temperature-dependent radiation-enhanced diffusion in ion-bombarded solids. , 1988, Physical review letters.

[18]  M. Toulemonde,et al.  Induced damage by high energy heavy ion irradiation at the GANIL accelerator in semiconductor materials , 1992 .

[19]  R. Yen,et al.  Femtosecond-Time-Resolved Surface Structural Dynamics of Optically Excited Silicon , 1983 .

[20]  R. S. Nelson An investigation of thermal spikes by studying the high energy sputtering of metals at elevated temperatures , 1965 .

[21]  G. Betz,et al.  Studies of surface composition of Ag‐Au, Au‐Cu, and Ag‐Cu alloys after ion bombardment by Auger electron spectroscopy , 1977 .

[22]  B. Tsaur,et al.  Supersaturated metastable Ag-Ni solid solutions formed by ion beam mixing , 1980 .

[23]  I. Baranov,et al.  Inelastic sputtering of solids by ions , 1988 .

[24]  R. Kelly Thermal effects in sputtering , 1979 .

[25]  C. Chien,et al.  Observation of very-short-lived radiation effects in rare-earth solids following Coulomb excitation , 1979 .

[26]  Yuzhen Sun,et al.  Observation of post-bombardment segregation in an Au−Cu alloy at room temperature , 1986 .

[27]  O. Auciello,et al.  Ion Bombardment Modification of Surfaces: Fundamentals and Applications , 1984 .

[28]  A. Miotello,et al.  Ion-beam mixing with chemical guidance part III: phase formation as a kinetic rather than thermodynamic phenomenon , 1994 .

[29]  Meftah,et al.  Track formation in SiO2 quartz and the thermal-spike mechanism. , 1994, Physical review. B, Condensed matter.

[30]  Dufour,et al.  Transient thermal process after a high-energy heavy-ion irradiation of amorphous metals and semiconductors. , 1992, Physical review. B, Condensed matter.

[31]  H. Dammak,et al.  α→ω phase transformation induced in titanium during ion irradiations in the electronic slowing-down regime , 1993 .

[32]  M. W. Thompson,et al.  The effect of ion mass and target temperature on the energy distribution of sputtered atoms , 1980 .

[33]  W. Johnson,et al.  Influence of chemical driving forces in ion mixing of metallic bilayers , 1984 .

[34]  K. Kopitzki,et al.  Metastable phases formed by ion beam mixing of binary metal systems with positive heats of formation , 1988 .

[35]  W. Husinsky,et al.  Doppler shift laser fluorescence spectroscopy of sputtered and evaporated atoms under Ar+ bombardment , 1985 .

[36]  T. Wada,et al.  Complex defects introduced into Si by high‐energy electron irradiation: Production rates of defects in n‐Si , 1977 .

[37]  U. Littmark,et al.  A search for a thermal spike effect in sputtering. I. Temperature dependence of the yield at low-kev, heavy-ion bombardment , 1982 .

[38]  A. Miotello,et al.  Thermodynamic effects on ion-beam mixing in SiC–metal systems , 1994 .

[39]  G. Martin Phase stability under irradiation: Ballistic effects , 1984 .

[40]  A. Traverse,et al.  Quantitative Description of Mixing with Light Ions , 1989 .

[41]  A. G. Cullis,et al.  Transitions to Defective Crystal and the Amorphous State Induced in Elemental Si by Laser Quenching , 1982 .

[42]  W. O. Hofer,et al.  A search for a thermal spike effect in sputtering , 1983 .

[43]  R. Averback,et al.  Effect of viscous flow on ion damage near solid surfaces. , 1994, Physical review letters.

[44]  L. Hobbs Radiation damage in electron microscopy of inorganic solids , 1978 .

[45]  Josef Michl,et al.  A gas-flow model for the sputtering of condensed gases , 1987 .

[46]  J. Fine,et al.  Interface width dependence on sample temperature during Auger sputter depth profiling of Cr/Ni multilayered thin films , 1992 .

[47]  K. Hardy,et al.  OBSERVATION OF TEMPERATURE SPIKES FOLLOWING COULOMB EXCITATION. , 1972 .

[48]  R. Averback,et al.  Latent Tracks Do Exist in Metallic Materials , 1991 .

[49]  Fuchs,et al.  Evidence for amorphization of a metallic alloy by ion electronic energy loss. , 1990, Physical review letters.

[50]  M. Buchgeister,et al.  Ion beam mixing of selected binary metal systems with large positive heats of formation , 1989 .

[51]  J. Duraud,et al.  Swift heavy ion amorphization of quartz — a comparative study of the particle amorphization mechanism of quartz , 1996 .

[52]  M. H. Battey,et al.  Book Review: Nuclear tracks in solids: Principles and applications. R. L. FLEISCHER, P.B. PRICE and R.M. WALKER. University of California Press, 1975, 629 pp., $31.50 , 1976 .

[53]  S. Myers ION-BEAM-INDUCED MIGRATION AND ITS EFFECT ON CONCENTRATION PROFILES* , 1979 .

[54]  A. Miotello,et al.  Reply to “Comment on ‘Ion-beam mixing with chemical guidance. IV. Thermodynamic effects without invoking thermal spikes’ by D. Marton and J. Fine” , 1995 .

[55]  Roger Kelly,et al.  Thermal sputtering as a gas-dynamic process , 1990 .

[56]  A. Miotello,et al.  Ion-beam mixing with chemical guidance. IV: Thermodynamic effects without invoking thermal spikes , 1994 .

[57]  King,et al.  Role of thermal spikes in energetic displacement cascades. , 1987, Physical review letters.

[58]  Roger Kelly,et al.  Laser irradiation effects in Si+-implanted SiO2 , 1992 .

[59]  E. H. Hasseltine,et al.  Cesium‐Ion Bombardment of Aluminum Oxide in a Controlled Oxygen Environment , 1967 .