Abstract
The nature of the motion of charge carriers is reflected in the temperature dependence of their mobility. Photo-injected carriers in aromatic hydrocarbon crystals had shown puzzling behavior particularly in naphthalene in which the mobility drops with an increase in temperature from 30 to 100 K and is then unaffected by it as temperature varies further from 100 to 300 K. Many theories had been developed to explain the phenomenon. The chapter showed how they all fail when put to quantitative test. These qualitatively (apparently) successful explanations included standard acoustic phonon scattering formalisms, SLE considerations, and polaron considerations as well. It was shown how the GME theory with its specific calculational scheme applied to a system of polaronic transfer finally succeeded for the entire temperature interval and in all crystallographic considerations. Further calculations, some of them about the saturation of mobility with increasing field, and others designed to address materials with carrier bands broader than in narrow-band polaronic materials were developed. The latter showed how a mobility dependence could arise with the appearance of a band-hopping transition for intermediate width bands.
Access this chapter
Tax calculation will be finalised at checkout
Purchases are for personal use only
Notes
- 1.
The last two of the publications mentioned provided visually impressive quantitative fits of the theory to the data as well.
- 2.
Throughout my scientific life I have wondered what precisely “essential” means in this context. When do I know I have captured the essence of a problem through my theory? Did Einstein capture the essence in his theory of specific heats of insulators based on dispersionless oscillators? Does Debye’s innovation in this subject address an essential ingredient or is it a “mere matter of detail”? Is knowing whether one’s theory has captured the essence of an experiment an inner phenomenon only? Are there no criteria more objective than for knowing if one has fallen in love?
- 3.
In this chapter we show all occurrences of ħ explicitly to avoid any confusion because of the plentiful discussion of experimental data here.
- 4.
David Dunlap who collaborated on this fitting did not work further on crystal mobilities. He went on to produce, in collaboration with Paul Parris, a remarkable theory of the field-dependence of mobilities in the presence of dipolar disorder that will be mentioned passingly in Chap. 13 (Dunlap et al. 1996, 1999; Novikov et al. 1998; Kenkre et al. 1998a; Parris et al. 2001b). It has not been described in this book because it does not fit in with the flow of the book’s topics. However, I heartily recommend to the interested reader that fine work by Dunlap and Parris on the description of carrier transport in statically disordered systems.
- 5.
They went on to remark (Swenberg and Pope 1998) that “This surprisingly close agreement between the two approaches strengthens the validity of each...”.
- 6.
The late Larry Schein said to me when I asked him to push the measurements to that region, “I would if I could but the *&%*%&crystal melts at that point.”
- 7.
I find this topic powerful but personally rather mystifying and beset with logic that, to my uneducated eye, appears a tad confusing.
- 8.
Cautionary conclusions of this kind were also drawn by Conwell and Basko (2003) on independent grounds.
- 9.
This B to B 2 transition as temperature increases is reminiscent of the V to V 2 behavior we discussed in the Perrin-Förster problem of excitation transfer in Chap. 3 but arises here from a completely different source!
- 10.
We have kept to the definition of B here used in Kenkre (2002) rather than in Kenkre et al. (1989) although there is unfortunately a discrepancy of a factor of 4 in the two. B is simply the assumed matrix element V in the tightbinding model in the former but the actual bandwidth that results from it in the latter. Quantitative precision is not being sought here and I hope my pointing this out will help rather than harm the explanations.
- 11.
It was unfortunately not pursued further because of the data falsification situation in the field alluded to earlier. I believe that serious theoretical analysis should return with renewed intensity now that the field appears to have bounced back again under the leadership of inspired scientists such as Biscarini, Dodabalapur, and their collaborators. See, e.g., Cramer et al. (2009), Shehu et al. (2010), Wang and Dodabalapur (2018), Wang et al. (2019), and Wang and Dodabalapur (2020).
References
Andersen, J. D., Duke, C. B., & Kenkre, V. M. (1983). Injected electrons in naphthalene: Band motion at low temperatures. Physical Review Letters, 51(24), 2202.
Andersen, J. D., Duke, C. B., & Kenkre, V. M. (1984). Application of the Silbey-Munn theory to interpret the temperature dependence of the mobilities of injected electrons in naphthalene. Chemical Physics Letters, 110(5), 504–507.
Anderson, P. W. (1997). Concepts in solids: Lectures on the theory of solids (Vol. 58). River Edge, NJ: World Scientific.
Brown, D. W, Lindenberg, K., & Zhao, Y. (1997). Variational energy band theory for polarons: Mapping polaron structure with the global-local method. The Journal of Chemical Physics, 107(8), 3179–3195.
Cheng, Y.-C., & Silbey, R. J. (2008). A unified theory for charge-carrier transport in organic crystals. The Journal of Chemical Physics, 128(11), 114713.
Conwell, E. M., & Basko, D. M. (2003). Negative differential mobility in pentacene. Journal of Polymer Science Part B: Polymer Physics, 41(21), 2595–2600.
Cramer, T., Steinbrecher, T., Koslowski, T., Case, D. A., Biscarini, F., & Zerbetto, F. (2009). Water-induced polaron formation at the pentacene surface: Quantum mechanical molecular mechanics simulations. Physical Review B, 79(15), 155316.
Duke, C. B, & Schein, L. B. (1980). Organic solids: Is energy-band theory enough? Physics Today, 33(2), 42–48.
Dunlap, D. H., & Kenkre, V. M. (1993). Disordered polaron transport: A theoretical description of the motion of photoinjected charges in molecularly doped polymers. Chemical Physics, 178, 67–75.
Dunlap, D. H., Kenkre, V. M., & Parris, P. E. (1999). What is behind the square root of E? Journal of Imaging Science and Technology, 43(5), 437–443.
Dunlap, D. H., Parris, P. E., & Kenkre, V. M. (1996). Charge-dipole model for the universal field dependence of mobilities in molecularly doped polymers. Physical Review Letters, 77(3), 542.
Efrima, S., & Metiu, H. (1979). The temperature dependence of the electron mobility in molecular crystals. Chemical Physics Letters, 60(2), 226–231.
Erginsoy, C. (1950). Neutral impurity scattering in semiconductors. Physical Review, 79(6), 1013.
Giuggioli, L., Andersen, J. D., & Kenkre, V. M. (2003). Mobility theory of intermediate-bandwidth carriers in organic crystals: Scattering by acoustic and optical phonons. Physical Review B, 67(4), 045110.
Grover, M., & Silbey, R. (1971). Exciton migration in molecular crystals. The Journal of Chemical Physics, 54(11), 4843–4851.
Harris, R. A., & Silbey, R. (1985). Variational calculation of the tunneling system interacting with a heat bath. II. Dynamics of an asymmetric tunneling system. The Journal of Chemical Physics, 83(3), 1069–1074.
Kenkre, V. M. (1975c). Relations among theories of excitation transfer. II. Influence of spectral features on exciton motion. Physical Review B, 12(6), 2150.
Kenkre, V. M. (2002). Finite-bandwidth calculations for charge carrier mobility in organic crystals. Physics Letters A, 305(6), 443–447.
Kenkre, V. M., Andersen, J. D., Dunlap, D. H., & Duke, C. B. (1989). Unified theory of the mobilities of photoinjected electrons in naphthalene. Physical Review Letters, 62(10), 1165.
Kenkre, V. M., & Lindenberg, K. (2003). Modern challenges in statistical mechanics: Patterns, noise, and the interplay of nonlinearity and complexity. In Conference Proceedings (Vol. 658). Melville, NY: American Institute of Physics.
Kenkre, V. M., & Parris, P. E. (2002a). Mechanism for carrier velocity saturation in pure organic crystals. Physical Review B, 65(24), 245106.
Kenkre, V. M., & Parris, P. E. (2002b). Saturation of charge carrier velocity with increasing electric fields: Theoretical investigations for pure organic crystals. Physical Review B, 65(20), 205104.
Kenkre, V. M., Scott, J. E., Pease, E. A., & Hurd, A. J. (1998a). Nonlocal approach to the analysis of the stress distribution in granular systems. I. Theoretical framework. Physical Review E, 57(5), 5841–5849.
Madhukar, A., & Post, W. (1977). Exact solution for the diffusion of a particle in a medium with site diagonal and off-diagonal dynamic disorder. Physical Review Letters, 39(22), 1424.
Merrifield, R. E. (1964). Theory of the vibrational structure of molecular exciton states. The Journal of Chemical Physics, 40(2), 445–450.
Nasu, K., & Toyozawa, Y. (1981). Tunneling process from free state to self-trapped state of exciton. Journal of the Physical Society of Japan, 50(1), 235–245.
Novikov, S. V., Dunlap, D. H., Kenkre, V. M., Parris, P. E., & Vannikov, A. V. (1998). Essential role of correlations in governing charge transport in disordered organic materials. Physical Review Letters, 81(20), 4472.
Parris, P. E., & Kenkre, V. M. (2004). Variational considerations in the study of carrier transport in organic crystals. Physical Review B, 70(6), 064304.
Parris, P. E., Kenkre, V. M., & Dunlap, D. H. (2001b). Nature of charge carriers in disordered molecular solids: Are polarons compatible with observations? Physical Review Letters, 87(12), 126601.
Parris, P. E., Kuś, M., & Kenkre, V. M. (2001a). Fokker–Planck analysis of the nonlinear field dependence of a carrier in a band at arbitrary temperatures. Physics Letters A, 289(4–5), 188–192.
Parris, P. E., & Silbey, R. (1985). Low temperature tunneling dynamics in condensed media. The Journal of Chemical Physics, 83(11), 5619–5626.
Pope, M., & Swenberg, C. E. (1999). Electronic processes in organic crystals and polymers (2nd ed.) New York: Oxford University Press.
Reineker, P., Kenkre, V. M., & Kühne, R. (1981). Drift mobility of photo-electrons in organic molecular crystals: Quantitative comparison between theory and experiment. Physics Letters A, 84(5), 294–296.
Roberts, G. G., Apsley, N., & Munn, R. W. (1980). Temperature dependent electronic conduction in semiconductors. Physics Reports, 60(2), 59–150.
Schein, L. B., Duke, C. B., & McGhie, A. R. (1978). Observation of the band-hopping transition for electrons in naphthalene. Physical Review Letters, 40(3), 197.
Shehu, A., Quiroga, S. D., D’Angelo, P., Albonetti, C., Borgatti, F., Murgia, M., et al. (2010). Layered distribution of charge carriers in organic thin film transistors. Physical Review Letters, 104(24), 246602.
Silbey, R. (1976). Electronic energy transfer in molecular crystals. Annual Review of Physical Chemistry, 27(1), 203–223.
Silbey, R., & Harris, R. A. (1984). Variational calculation of the dynamics of a two level system interacting with a bath. The Journal of Chemical Physics, 80(6), 2615–2617.
Silbey, R., & Munn, R. W. (1980). General theory of electronic transport in molecular crystals. I. Local linear electron–phonon coupling. The Journal of Chemical Physics, 72(4), 2763–2773.
E. A. Silinsh & V. Capek (Eds.) (1994). Organic electronic materials-interaction, localization and transport phenomena. New York: American Institute of Physics.
Sumi, H. (1979a). Theory of electrical conduction in organic molecular crystals. II. Characteristic effects of electric field and defect scattering on temperature-independent mobilities. The Journal of Chemical Physics, 71(8), 3403–3411.
Sumi, H. (1979b). Theory of electrical conduction in organic molecular crystals: Temperature-independent mobilities. The Journal of Chemical Physics, 70(8), 3775–3785.
Swenberg, C. E., & Pope, M. (1998). An observation on the mobility and the carrier effective mass in naphthalene. Chemical Physics Letters, 287(5–6), 535–536.
Wang, X., & Dodabalapur, A. (2018). Trapped carrier scattering and charge transport in high-mobility amorphous metal oxide thin-film transistors. Annalen der Physik, 530(12), 1800341.
Wang, X., & Dodabalapur, A. (2020). Going beyond polaronic theories in describing charge transport in rubrene single crystals. Applied Physics Letters, 116(9), 093301.
Wang, X., Register, L. F., & Dodabalapur, A. (2019). Redefining the mobility edge in thin-film transistors. Physical Review Applied, 11(6), 064039.
Warta, W., & Karl, N. (1985). Hot holes in naphthalene: High, electric-field-dependent mobilities. Physical Review B, 32(2), 1172.
Wu, M. W., & Conwell, E. M. (1997). Transport in α-sexithiophene films. Chemical Physics Letters, 266(3–4), 363–367.
Yarkony, D. R., & Silbey, R. (1977). Variational approach to exciton transport in molecular crystals. The Journal of Chemical Physics, 67(12), 5818–5827.
Author information
Authors and Affiliations
Rights and permissions
Copyright information
© 2021 The Author(s), under exclusive license to Springer Nature Switzerland AG
About this chapter
Cite this chapter
Kenkre, V.M.(. (2021). Application to Charges Moving in Crystals: Resolution of the Mobility Puzzle in Naphthalene and Related Results. In: Memory Functions, Projection Operators, and the Defect Technique. Lecture Notes in Physics, vol 982. Springer, Cham. https://doi.org/10.1007/978-3-030-68667-3_6
Download citation
DOI: https://doi.org/10.1007/978-3-030-68667-3_6
Published:
Publisher Name: Springer, Cham
Print ISBN: 978-3-030-68666-6
Online ISBN: 978-3-030-68667-3
eBook Packages: Physics and AstronomyPhysics and Astronomy (R0)