Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Effect of Glass Stability on the Low Frequency Vibrations of Vapor Deposited Glasses

I. Festi1,*, E. Alfinelli1, D. Bessas2, F. Caporaletti3, A. I. Chumakov2, M. Moratalla4, M. A. Ramos4, M. Rodríguez-López5,6, C. Rodríguez-Tinoco5,6 et al.

J. Rodríguez-Viejo5,6 and G. Baldi1,†

  • *Contact author: irene.festi@unitn.it
  • †Contact author: giacomo.baldi@unitn.it

Phys. Rev. X 16, 021021 – Published 28 April, 2026

DOI: https://doi.org/10.1103/311v-1ftn

Abstract

Ultrastable glasses prepared from the physical vapor deposition of organic molecules present a very low density of two-level states, the kind of glass defects that determine their peculiar low-temperature thermal properties. Numerical simulations suggest that quasilocalized harmonic vibrational modes emerge in the soft regions associated with two-level states. However, the connection between the low-frequency vibrational modes and the local structural instabilities of glasses remains unexplained. Here, we exploit a recently developed spectrograph for nuclear resonant analysis of inelastic x-ray scattering to probe the density of vibrational states of amorphous thin films of ultrastable and conventional glasses down to an exceptionally low frequency of approximately 70 GHz. We show that the glass stability does not affect the harmonic vibrational modes at the lowest frequencies, despite a reduction of almost an order of magnitude in the density of two-level states. At the same time, the vibrational modes at higher frequencies, around the boson peak maximum, are extremely sensitive to the glass stability. Although we cannot exclude the possible existence of quasilocalized modes in glasses, we show that their presence is not strictly necessary to describe the measured density of low-frequency vibrations. The experimental developments here presented pave the way to the solution to the long-standing debate on the low-frequency vibrations in glasses.

View figure in article

Physics Subject Headings (PhySH)

Popular Summary

Article Text

References (80)

  1. P. G. Debenedetti and F. H. Stillinger, Supercooled liquids and the glass transition, Nature (London) 410, 259 (2001).
  2. R. C. Zeller and R. O. Pohl, Thermal conductivity and specific heat of noncrystalline solids, Phys. Rev. B 4, 2029 (1971).
  3. W. A. Phillips, Two-level states in glasses, Rep. Prog. Phys. 50, 1657 (1987).
  4. J. C. Chan, A. D. Rakic, C. Y. Kwong, A. B. Djurisic, M. L. Majewski, W. K. Chan, and P. C. Chui, Optimization of organic light emitting diode structures, in Photonics: Design, Technology, and Packaging, edited by C. Jagadish, K. D. Choquette, B. J. Eggleton, B. D. Nener, and K. A. Nugent (SPIE, Bellingham, WA, 2004), Vol. 5277, p. 311.
  5. J. Song, H. Lee, E. G. Jeong, K. C. Choi, and S. Yoo, Organic light-emitting diodes: Pushing toward the limits and beyond, Adv. Mater. 32, 1907539 (2020).
  6. A. J. Addie, R. A. Ismail, and M. A. Mohammed, Amorphous carbon nitride dual-function anti-reflection coating for crystalline silicon solar cells, Sci. Rep. 12, 9902 (2022).
  7. M. R. Abernathy, X. Liu, and T. H. Metcalf, An overview of research into low internal friction optical coatings by the gravitational wave detection community, Mater. Res. 21, e20170863 (2018).
  8. S. F. Swallen, K. L. Kearns, M. K. Mapes, Y. S. Kim, R. J. McMahon, M. D. Ediger, T. Wu, L. Yu, and S. Satija, Organic glasses with exceptional thermodynamic and kinetic stability, Science 315, 353 (2007).
  9. C. Rodriguez-Tinoco, M. Gonzalez-Silveira, M. A. Ramos, and J. Rodriguez-Viejo, Ultrastable glasses: New perspectives for an old problem, Riv. Nuovo Cimento 45, 325 (2022).
  10. T. Pérez-Castañeda, C. Rodríguez-Tinoco, J. Rodríguez-Viejo, and M. A. Ramos, Suppression of tunneling two-level systems in ultrastable glasses of indomethacin, Proc. Natl. Acad. Sci. U.S.A. 111, 11275 (2014).
  11. M. Moratalla, M. Rodríguez-López, C. Rodríguez-Tinoco, J. Rodríguez-Viejo, R. J. Jiménez-Riobóo, and M. A. Ramos, Depletion of two-level systems in highly stable glasses with different molecular ordering, Commun. Phys. 6, 274 (2023).
  12. L. Berthier and M. D. Ediger, Facets of glass physics, Phys. Today 69, No. 1, 40 (2016).
  13. G. Baldi, A. Fontana, and G. Monaco, Vibrational dynamics of non-crystalline solids, in Low-Temperature Thermal and Vibrational Properties of Disordered Solids (World Scientific, Singapore, 2022) Chap. 6, pp. 177–226.
  14. V. G. Karpov, M. I. Klinger, and F. N. Ignatiev, Theory of the low-temperature anomalies in the thermal properties of amorphous structures, Sov. Phys. JETP 57, 439 (1983).
  15. U. Buchenau, Y. M. Galperin, V. L. Gurevich, and H. R. Schober, Anharmonic potentials and vibrational localization in glasses, Phys. Rev. B 43, 5039 (1991).
  16. S. N. Taraskin, Y. L. Loh, G. Natarajan, and S. R. Elliott, Origin of the boson peak in systems with lattice disorder, Phys. Rev. Lett. 86, 1255 (2001).
  17. T. S. Grigera, V. Martín-Mayor, G. Parisi, and P. Verrocchio, Phonon interpretation of the ‘boson peak’ in supercooled liquids, Nature (London) 422, 289 (2003).
  18. D. A. Parshin, H. R. Schober, and V. L. Gurevich, Vibrational instability, two-level systems, and the boson peak in glasses, Phys. Rev. B 76, 064206 (2007).
  19. W. Schirmacher, G. Ruocco, and T. Scopigno, Acoustic attenuation in glasses and its relation with the boson peak, Phys. Rev. Lett. 98, 025501 (2007).
  20. B. Rufflé, D. A. Parshin, E. Courtens, and R. Vacher, Boson peak and its relation to acoustic attenuation in glasses, Phys. Rev. Lett. 100, 015501 (2008).
  21. A. I. Chumakov et al., Role of disorder in the thermodynamics and atomic dynamics of glasses, Phys. Rev. Lett. 112, 025502 (2014).
  22. E. DeGiuli, A. Laversanne-Finot, G. Düring, E. Lerner, and M. Wyart, Effects of coordination and pressure on sound attenuation, boson peak and elasticity in amorphous solids, Soft Matter 10, 5628 (2014).
  23. M. Baggioli, R. Milkus, and A. Zaccone, Vibrational density of states and specific heat in glasses from random matrix theory, Phys. Rev. E 100, 062131 (2019).
  24. M. González-Jiménez, T. Barnard, B. A. Russell, N. V. Tukachev, U. Javornik, L.-A. Hayes, A. J. Farrell, S. Guinane, H. M. Senn, A. J. Smith, M. Wilding, G. Mali, M. Nakano, Y. Miyazaki, P. McMillan, G. C. Sosso, and K. Wynne, Understanding the emergence of the boson peak in molecular glasses, Nat. Commun. 14, 215 (2023).
  25. F. Vogel and M. Fuchs, Vibrational phenomena in glasses at low temperatures captured by field theory of disordered harmonic oscillators, Phys. Rev. Lett. 130, 236101 (2023).
  26. C. Jiang, M. Baggioli, and J. F. Douglas, Stringlet excitation model of the boson peak, J. Chem. Phys. 160, 214505 (2024).
  27. Y.-C. Hu and H. Tanaka, Origin of the boson peak in amorphous solids, Nat. Phys. 18, 669 (2022).
  28. L. Wang, A. Ninarello, P. Guan, L. Berthier, G. Szamel, and E. Flenner, Low-frequency vibrational modes of stable glasses, Nat. Commun. 10, 26 (2019).
  29. D. Khomenko, C. Scalliet, L. Berthier, D. R. Reichman, and F. Zamponi, Depletion of two-level systems in ultrastable computer-generated glasses, Phys. Rev. Lett. 124, 225901 (2020).
  30. D. Khomenko, D. R. Reichman, and F. Zamponi, Relationship between two-level systems and quasilocalized normal modes in glasses, Phys. Rev. Mater. 5, 055602 (2021).
  31. S. Ciarella, D. Khomenko, L. Berthier, F. C. Mocanu, D. R. Reichman, C. Scalliet, and F. Zamponi, Finding defects in glasses through machine learning, Nat. Commun. 14, 4229 (2023).
  32. D. Xu, S. Zhang, H. Tong, L. Wang, and N. Xu, Low-frequency vibrational density of states of ordinary and ultra-stable glasses, Nat. Commun. 15, 1424 (2024).
  33. E. Lerner, G. Düring, and E. Bouchbinder, Statistics and properties of low-frequency vibrational modes in structural glasses, Phys. Rev. Lett. 117, 035501 (2016).
  34. L. Angelani, M. Paoluzzi, G. Parisi, and G. Ruocco, Probing the non-Debye low-frequency excitations in glasses through random pinning, Proc. Natl. Acad. Sci. U.S.A. 115, 8700 (2018).
  35. H. Mizuno, H. Shiba, and A. Ikeda, Continuum limit of the vibrational properties of amorphous solids, Proc. Natl. Acad. Sci. U.S.A. 114, E9767 (2017).
  36. N. S. Shcheblanov, M. E. Povarnitsyn, J. D. Wiles, S. R. Elliott, and S. N. Taraskin, Phonon traces in glassy vibrations, Phys. Rev. B 102, 024202 (2020).
  37. D. Richard, K. González-López, G. Kapteijns, R. Pater, T. Vaknin, E. Bouchbinder, and E. Lerner, Universality of the nonphononic vibrational spectrum across different classes of computer glasses, Phys. Rev. Lett. 125, 085502 (2020).
  38. S. Bonfanti, R. Guerra, C. Mondal, I. Procaccia, and S. Zapperi, Universal low-frequency vibrational modes in silica glasses, Phys. Rev. Lett. 125, 085501 (2020).
  39. P. Das and I. Procaccia, Universal density of low-frequency states in amorphous solids at finite temperatures, Phys. Rev. Lett. 126, 085502 (2021).
  40. E. Lerner and E. Bouchbinder, Boson-peak vibrational modes in glasses feature hybridized phononic and quasilocalized excitations, J. Chem. Phys. 158, 194503 (2023).
  41. W. Schirmacher, M. Paoluzzi, F. C. Mocanu, D. Khomenko, G. Szamel, F. Zamponi, and G. Ruocco, The nature of non-phononic excitations in disordered systems, Nat. Commun. 15, 3107 (2024).
  42. E. Flenner and G. Szamel, Defects, sound damping, and the boson peak in amorphous solids, J. Phys. Chem. B 129, 1855 (2025).
  43. E. Flenner and G. Szamel, The origin of sound damping in amorphous solids: Defects and beyond, Sci. Adv. 11, eadu6097 (2025).
  44. A. I. Chumakov, Y. Shvyd’ko, I. Sergueev, D. Bessas, and R. Rüffer, Hard-X-ray spectroscopy with a spectrographic approach, Phys. Rev. Lett. 123, 097402 (2019).
  45. W. Schirmacher, C. Tomaras, B. Schmid, G. Baldi, G. Viliani, G. Ruocco, and T. Scopigno, Sound attenuation and anharmonic damping in solids with correlated disorder, Condens. Matter Phys. 13, 23606 (2010).
  46. W. Schirmacher, T. Scopigno, and G. Ruocco, Theory of vibrational anomalies in glasses, J. Non-Cryst. Solids 407, 133 (2015).
  47. Z. Pan, O. Benzine, S. Sawamura, R. Limbach, A. Koike, T. D. Bennett, G. Wilde, W. Schirmacher, and L. Wondraczek, Disorder classification of the vibrational spectra of modern glasses, Phys. Rev. B 104, 134106 (2021).
  48. J. Jäckle, Low frequency raman scattering in glasses, in Amorphous Solids: Low-Temperature Properties, edited by W. A. Phillips (Springer, Berlin, Heidelberg, 1981), pp. 135–160.
  49. U. Buchenau, N. Nücker, and A. J. Dianoux, Neutron scattering study of the low-frequency vibrations in vitreous silica, Phys. Rev. Lett. 53, 2316 (1984).
  50. E. Fabiani, A. Fontana, and U. Buchenau, Neutron scattering study of the vibrations in vitreous silica and germania, J. Chem. Phys. 128, 244507 (2008).
  51. X. Monnier, J. Colmenero, M. Wolf, and D. Cangialosi, Reaching the ideal glass in polymer spheres: Thermodynamics and vibrational density of states, Phys. Rev. Lett. 126, 118004 (2021).
  52. A. I. Chumakov et al., Role of disorder in the thermodynamics and atomic dynamics of glasses, Phys. Rev. Lett. 112, 025502 (2014).
  53. A. I. Chumakov, A. Q. R. Baron, R. Rüffer, H. Grünsteudel, H. F. Grünsteudel, and A. Meyer, Nuclear resonance energy analysis of inelastic X-ray scattering, Phys. Rev. Lett. 76, 4258 (1996).
  54. A. Chumakov and W. Sturhahn, Experimental aspects of inelastic nuclear resonance scattering, Hyperfine Interact. 123–124, 781 (1999).
  55. U. Buchenau, H. M. Zhou, N. Nucker, K. S. Gilroy, and W. A. Phillips, Structural relaxation in vitreous silica, Phys. Rev. Lett. 60, 1318 (1988).
  56. U. Buchenau, A. Wischnewski, M. Ohl, and E. Fabiani, Neutron scattering evidence on the nature of the boson peak, J. Phys. Condens. Matter 19, 205106 (2007).
  57. S. Caponi, A. Fontana, F. Rossi, G. Baldi, and E. Fabiani, Effect of temperature on the vibrational density of states in vitreous SiO2: A Raman study, Phys. Rev. B 76, 092201 (2007).
  58. G. Baldi, V. M. Giordano, B. Ruta, R. Dal Maschio, A. Fontana, and G. Monaco, Anharmonic damping of terahertz acoustic waves in a network glass and its effect on the density of vibrational states, Phys. Rev. Lett. 112, 125502 (2014).
  59. Q. Ren et al., Extreme phonon anharmonicity underpins superionic diffusion and ultralow thermal conductivity in argyrodite Ag8SnSe6, Nat. Mater. 22, 999 (2023).
  60. U. Buchenau, The soft-potential model and its extensions, in Low-Temperature Thermal and Vibrational Properties of Disordered Solids (World Scientific, Singapore, 2022), Chap. 8, pp. 299–330.
  61. M. A. Ramos, Low-temperature specific heat of glasses and disordered crystals, in Low-Temperature Thermal and Vibrational Properties of Disordered Solids (World Scientific, Singapore, 2022), Chap. 2, pp. 21–67.
  62. A. Moriel, E. Lerner, and E. Bouchbinder, Boson peak in the vibrational spectra of glasses, Phys. Rev. Res. 6, 023053 (2024).
  63. A. Moriel, E. Lerner, and E. Bouchbinder, Experimental evidence for the ω4 tail of the nonphononic spectra of glasses, J. Appl. Phys. 136, 225105 (2024).
  64. A. Gujral, K. A. O’Hara, M. F. Toney, M. L. Chabinyc, and M. D. Ediger, Structural characterization of vapor-deposited glasses of an organic hole transport material with X-ray scattering, Chem. Mater. 27, 3341 (2015).
  65. J. Ràfols-Ribé, R. Dettori, P. Ferrando-Villalba, M. Gonzalez-Silveira, L. Abad, A. F. Lopeandía, L. Colombo, and J. Rodríguez-Viejo, Evidence of thermal transport anisotropy in stable glasses of vapor deposited organic molecules, Phys. Rev. Mater. 2, 035603 (2018).
  66. M. A. Ramos, C. Talón, and S. Vieira, The boson peak in structural and orientational glasses of simple alcohols: Specific heat at low temperatures, J. Non-Cryst. Solids 307–310, 80 (2002).
  67. S. Singh, M. D. Ediger, and J. J. de Pablo, Ultrastable glasses from in silico vapour deposition, Nat. Mater. 12, 139 (2013).
  68. L. Gil, M. A. Ramos, A. Bringer, and U. Buchenau, Low-temperature specific heat and thermal conductivity of glasses, Phys. Rev. Lett. 70, 182 (1993).
  69. I. Festi, M. Rodríguez-López, C. Rodríguez-Tinoco, J. Rodríguez-Viejo, F. Rossi, and G. Baldi, Raman spectroscopy of an ultrastable glass, Philos. Mag. (2025), 10.1080/14786435.2025.2547672.
  70. G. Baldi, V. M. Giordano, G. Monaco, and B. Ruta, Sound attenuation at terahertz frequencies and the boson peak of vitreous silica, Phys. Rev. Lett. 104, 195501 (2010).
  71. B. Rufflé, G. Guimbretière, E. Courtens, R. Vacher, and G. Monaco, Glass-specific behavior in the damping of acousticlike vibrations, Phys. Rev. Lett. 96, 045502 (2006).
  72. D. Fainozzi, F. Caporaletti, F. Capotondi, D. De Angelis, R. A. Duncan, L. Foglia, A. Martinelli, R. Mincigrucci, K. A. Nelson, E. Pedersoli, M. Zanatta, A. A. Maznev, G. Monaco, F. Bencivenga, and G. Baldi, Temperature effects on the nanoscale thermoelastic response of a SiO2 membrane, APL Mater. 12, 051122 (2024).
  73. P.-J. Wang, A. Huynh, J.-K. Sheu, X. Lafosse, A. Lemaître, B. Rufflé, R. Vacher, B. Perrin, C.-K. Sun, and M. Foret, Quartic scaling of sound attenuation with frequency in vitreous silica, Phys. Rev. Lett. 134, 196101 (2025).
  74. https://zenodo.org/records/15448959.
  75. R. Rüffer and A. I. Chumakov, Nuclear resonance beamline at ESRF, Hyperfine Interact. 97–98, 589 (1996).
  76. A. I. Chumakov, A. Q. R. Baron, R. Rüffer, H. Grünsteudel, H. F. Grünsteudel, and A. Meyer, Nuclear resonance energy analysis of inelastic X-ray scattering, Phys. Rev. Lett. 76, 4258 (1996).
  77. V. Kohn and A. Chumakov, Dos: Evaluation of phonon density of states from nuclear resonant inelastic absorption, Hyperfine Interact. 125, 205 (2000).
  78. A. I. Chumakov, A. Bosak, and R. Rüffer, Contribution of acoustic modes to the density of vibrational states measured by inelastic scattering techniques, Phys. Rev. B 80, 094303 (2009).
  79. M. A. Ramos, L. Gil, A. Bringer, and U. Buchenau, The density of tunneling and vibrational states of glasses within the soft-potential model, Phys. Status Solidi (a) 135, 477 (1993).
  80. B. Schmid and W. Schirmacher, Raman scattering and the low-frequency vibrational spectrum of glasses, Phys. Rev. Lett. 100, 137402 (2008).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation