Glassy Anomalies in the Low-Temperature Thermal Properties of a Minimally Disordered Crystalline Solid

Gebbia, Jonathan F.; Ramos, M. A.; Szewczyk, Daria; Jeżowski, A.; Кривчиков, А. И.; Horbatenko, Yu. V.; Guidi, T.; Bermejo, Francisco Javier; Tamarit, J. Ll.

doi:10.1103/physrevlett.119.215506

Cited by 37 publications

(35 citation statements)

References 66 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…We also note that the low-energy optical phonons induce a scaling of the specific heat at low-T which approximately goes like C(T)∼T. While it is accepted that the specific heat in glasses goes linearly in T at low T, similar non-Debye glassy anomalies have been recently observed in crystals [14,17]. This finding can therefore help to shed new light on the origin of these glassy-like anomalies in the specific heat of crystals, where disordered-based TLS arguments are not applicable.…”

Section: Discussionsupporting

confidence: 77%

See 1 more Smart Citation

Low-energy optical phonons induce glassy-like vibrational and thermal anomalies in ordered crystals

Baggioli

Zaccone

2019

J. Phys. Mater.

View full text Add to dashboard Cite

It is widely accepted that structural glasses and disordered crystals exhibit anomalies in their thermal, mechanical and acoustic properties as manifestations of the breakdown of the long-wavelength approximation in a disordered dissipative environment. However, the same type of glassy-like anomalies (i.e. boson peak in the vibrational density of states (VDOS) above the Debye level, peak in the normalized specific heat at T;10 K etc) have been recently observed also in perfectly ordered crystals, including thermoelectric compounds. Here we present a theory that predicts these surprising effects in perfectly ordered crystals as a result of low-lying (soft) optical phonons. In particular, it is seen that a strong boson peak anomaly (low-energy excess of modes) in the VDOS can be due almost entirely to the presence of low-energy optical phonons, provided that their energy is comparable to that of the acoustic modes at the Brillouin zone boundary. The boson peak is predicted also to occur in the heat capacity at low T. In presence of strong damping (which might be due to anharmonicities in the ordered crystals), these optical phonons contribute to the low-T deviation from Debye's T 3 law, producing a linear-in-T behavior which is typical of glasses, even though no assumptions of disorder whatsoever are made in the model. These findings are relevant for understanding and tuning thermal transport properties of thermoelectric compounds, and possibly for the enhancement of electron-phonon superconductivity.

show abstract

Section: Discussionsupporting

confidence: 77%

“…Recent experimental works have demonstrated the existence of the very same anomalies (boson peak and heat capacity anomaly) also in perfectly ordered crystals, such as molecular single crystals [14][15][16] and noncentrosymmetric perfect crystals such as α-quartz [17].…”

Section: Introductionmentioning

confidence: 97%

Low-energy optical phonons induce glassy-like vibrational and thermal anomalies in ordered crystals

Baggioli

Zaccone

2019

J. Phys. Mater.

View full text Add to dashboard Cite

show abstract

“…Importance of thermal conductivity for investigating the effect of the nature of disorder on phonon propagation is currently a subject of interest, and several kinetically frozen ODICs have been studied, [48][49][50] and their features compared against those of glassy state of the same material. 49 It has also been used to study the vibrational density of states at low temperatures.…”

Section: Experimental Methodsmentioning

confidence: 99%

“…49 It has also been used to study the vibrational density of states at low temperatures. 50 We will discuss the effects on the features of other ODICs 31,32 and their Tog in Sect. IV.…”

Section: Experimental Methodsmentioning

confidence: 99%

Instability and thermal conductivity of pressure-densified and elastically altered orientational glass of Buckminsterfullerene

Johari

Andersson

Sundqvist

2018

The Journal of Chemical Physics

View full text Add to dashboard Cite

We report on the temperature, pressure, and time (T, p, and t)-dependent features of thermal conductivity, κ, of partially ordered, non-equilibrium state of C60-OG, the orientational glass of Buckminsterfullerene (at T below the orientational freezing temperature Tog) made more unstable (i) by partially depressurizing its high-p formed state to elastically expand it and (ii) by further pressurizing that state to elastically contract it. The sub-Tog effects observed on heating of C60-OG differ from those of glasses because phonon propagation depends on the ratio of two well-defined orientational states of C60 molecules and the density of the solid. A broad peak-like feature appears at T near Tog in the κ-T plots of C60-OG formed at 0.7 GPa, depressurized to 0.2 GPa and heated at 0.2 GPa, which we attribute to partial overlap of the sub-Tog and Tog features. A sub-Tog local minimum appears in the κ-T plots at T well below Tog of C60-OG formed at 0.1 GPa, pressurized to 0.5 GPa and heated at 0.5 GPa and it corresponds to the state of maximum disorder. Although Buckminsterfullerene is regarded as an orientationally disordered crystal, variation of its properties with T and p is qualitatively different from other such crystals. We discuss the findings in terms of the nature of its disorder, sensitivity of its rotational dynamics to temperature, and the absence of the Johari-Goldstein relaxation. All seem to affect the phenomenology of its glass-like transition.

show abstract

“…Interestingly, such universal dynamics of disordered materials also appears in a few single crystals. As discovered in recent studies, BPs or amorphous-like thermal behaviours appear in single crystals, such as thermoelectric materials [6][7][8][9] , pure relaxor materials 10 , and atypical organic materials 11,12 , and theoretical studies for elucidating anomalous phenomena are underway 8,[13][14][15] .…”

Section: Introductionmentioning

confidence: 96%

Detection of Boson Peak and Fractal Dynamics of Protein by Terahertz Time-Domain Spectroscopy

Mori

Jiang

Motoji

et al. 2018

2018 43rd International Conference on Infrared, Millimeter, and Terahertz Waves (IRMMW-THz)

View full text Add to dashboard Cite

Disordered systems exhibit universal excitation, referred to as the boson peak, in the terahertz region. Meanwhile, the so-called fracton is expected to appear in the nanoscale region owing to the self-similar structure of monomers in polymeric glasses. We demonstrate that such excitations can be detected using terahertz spectroscopy. For the interaction between terahertz light and the vibrational density of states of the fractal structure, we formulate an infrared light-vibration coupling coefficient for the fracton region. Accordingly, we show that information concerning fractal and fracton dimensions appears in the exponent of the absorption coefficient. Finally, using terahertz time-domain spectroscopy and low-frequency Raman scattering, we experimentally observe these universal excitations in a protein lysozyme system that has an intrinsically disordered and self-similar nature in a single supramolecule. These findings are applicable to disordered and polymeric glasses in general and will be key to understanding universal dynamics of disordered systems by terahertz light.

show abstract

Glassy Anomalies in the Low-Temperature Thermal Properties of a Minimally Disordered Crystalline Solid

Cited by 37 publications

References 66 publications

Low-energy optical phonons induce glassy-like vibrational and thermal anomalies in ordered crystals

Low-energy optical phonons induce glassy-like vibrational and thermal anomalies in ordered crystals

Instability and thermal conductivity of pressure-densified and elastically altered orientational glass of Buckminsterfullerene

Detection of Boson Peak and Fractal Dynamics of Protein by Terahertz Time-Domain Spectroscopy

Contact Info

Product

Resources

About