Low-temperature thermal conductivity of solid carbon dioxide

Preliminary results of the thermal conductivity measurements performed in the temperature range 1.5-35 K on pure carbon dioxide are presented. The data below 25 K have been obtained for the first time. The thermal conductivity coefficient reaches very high value, of about 700 W/(m×K), unusual for si...

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Дата:2003
Автори: Sumarokov, V.V., Stachowiak, P., Jezowski, A.
Формат: Стаття
Мова:English
Опубліковано: Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України 2003
Назва видання:Физика низких температур
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Онлайн доступ:https://nasplib.isofts.kiev.ua/handle/123456789/128853
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Цитувати:Low-temperature thermal conductivity of solid carbon dioxide / V.V. Sumarokov, P. Stachowiak, A. Jezowski // Физика низких температур. — 2003. — Т. 29, № 5. — С. 603-605. — Бібліогр.: 9 назв. — англ.

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Digital Library of Periodicals of National Academy of Sciences of Ukraine
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spelling nasplib_isofts_kiev_ua-123456789-1288532025-02-10T01:45:50Z Low-temperature thermal conductivity of solid carbon dioxide Sumarokov, V.V. Stachowiak, P. Jezowski, A. Динамика кристаллической решетки Preliminary results of the thermal conductivity measurements performed in the temperature range 1.5-35 K on pure carbon dioxide are presented. The data below 25 K have been obtained for the first time. The thermal conductivity coefficient reaches very high value, of about 700 W/(m×K), unusual for simple molecular crystal. Straightforward analysis applied to the data indicates the case of large-grained sample. 2003 Article Low-temperature thermal conductivity of solid carbon dioxide / V.V. Sumarokov, P. Stachowiak, A. Jezowski // Физика низких температур. — 2003. — Т. 29, № 5. — С. 603-605. — Бібліогр.: 9 назв. — англ. 0132-6414 PACS: 66.70.+f https://nasplib.isofts.kiev.ua/handle/123456789/128853 en Физика низких температур application/pdf Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України
institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
collection DSpace DC
language English
topic Динамика кристаллической решетки
Динамика кристаллической решетки
spellingShingle Динамика кристаллической решетки
Динамика кристаллической решетки
Sumarokov, V.V.
Stachowiak, P.
Jezowski, A.
Low-temperature thermal conductivity of solid carbon dioxide
Физика низких температур
description Preliminary results of the thermal conductivity measurements performed in the temperature range 1.5-35 K on pure carbon dioxide are presented. The data below 25 K have been obtained for the first time. The thermal conductivity coefficient reaches very high value, of about 700 W/(m×K), unusual for simple molecular crystal. Straightforward analysis applied to the data indicates the case of large-grained sample.
format Article
author Sumarokov, V.V.
Stachowiak, P.
Jezowski, A.
author_facet Sumarokov, V.V.
Stachowiak, P.
Jezowski, A.
author_sort Sumarokov, V.V.
title Low-temperature thermal conductivity of solid carbon dioxide
title_short Low-temperature thermal conductivity of solid carbon dioxide
title_full Low-temperature thermal conductivity of solid carbon dioxide
title_fullStr Low-temperature thermal conductivity of solid carbon dioxide
title_full_unstemmed Low-temperature thermal conductivity of solid carbon dioxide
title_sort low-temperature thermal conductivity of solid carbon dioxide
publisher Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України
publishDate 2003
topic_facet Динамика кристаллической решетки
url https://nasplib.isofts.kiev.ua/handle/123456789/128853
citation_txt Low-temperature thermal conductivity of solid carbon dioxide / V.V. Sumarokov, P. Stachowiak, A. Jezowski // Физика низких температур. — 2003. — Т. 29, № 5. — С. 603-605. — Бібліогр.: 9 назв. — англ.
series Физика низких температур
work_keys_str_mv AT sumarokovvv lowtemperaturethermalconductivityofsolidcarbondioxide
AT stachowiakp lowtemperaturethermalconductivityofsolidcarbondioxide
AT jezowskia lowtemperaturethermalconductivityofsolidcarbondioxide
first_indexed 2025-12-02T13:42:13Z
last_indexed 2025-12-02T13:42:13Z
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fulltext Fizika Nizkikh Temperatur, 2003, v. 29, No. 5, p. 603–605 Low-temperature thermal conductivity of solid carbon dioxide V.V. Sumarokov, P. Stachowiak, and A. Je¿owski Institute for Low Temperatures and Structure Research of the Polish Academy of Sciences P.O. Box 1410, 50-950 Wroc³aw, Poland E-mail: p_stach@int.pan.wroc.pl Received May 4, 2003 Preliminary results of the thermal conductivity measurements performed in the temperature range 1.5–35 K on pure carbon dioxide are presented. The data below 25 K have been obtained for the first time. The thermal conductivity coefficient reaches very high value, of about 700 W/(m�K), unusual for simple molecular crystal. Straightforward analysis applied to the data indicates the case of large-grained sample. PACS: 66.70.+f Solid carbon dioxide belongs to the group of simple molecular crystals formed from linear molecules (N2, CO, CO2 and N2O belong to the same group). At equilibrium vapor pressure CO2 crystal has unchanged fcc structure in the whole range of its existence [1,2]. In the solid phase the axes of O–C–O molecules, whose carbon atoms are located in the sites of the lat- tice, are oriented along space diagonals of the cubic elementary cell (Pa3 space group). Thermal, optical and other properties of solid CO2 have been studied over a wide range of temperature and pressure, see, e.g., [1,2] and references therein. However, the thermal conductivity at equilibrium va- por pressure was investigated only for temperatures above 27 K [3]. Extension of investigation of the ther- mal conductivity of solid CO2 towards lower tempera- tures is of interest by itself. Besides that, a comparison with the results obtained earlier for other simple mo- lecular crystals would provide new information con- cerning various internal processes in the crystals. This work presents preliminary results of measure- ments of the thermal conductivity of solid carbon di- oxide in the temperature range 1.5–36 K. Experimental The crystal of CO2 was grown, thermally treated and measured in the home-designed liquid He experi- mental setup, described fully in [4]. The central part of the setup is a cylindrical glass ampoule which, during the experiment, contains the sample under investigation. The ampoule, of length of 36 mm, has inner diameter of 4.2 mm and the wall thickness of 1 mm. Two germanium resistance ther- mometers are attached to the wall of the ampoule by means of thin cooper rings and heat-conducting glue. During measurements the thermometers serve the pur- pose of temperature and temperature gradient deter- mination. The distance between the thermometers is 12 mm and the lower thermometer is positioned � 9 mm from the bottom of the ampoule. The CO2 crystal was obtained from gas of natural isotopic composition and of 99.999% chemical purity; the purity of the gas was checked by means of a mass spectrometer. The sample of solid CO2 was grown from gaseous phase, starting at the bottom of the am- poule, with the following conditions of condensation: the temperature � 173.3 K, the pressure � 14 kPa, the growth rate � 1.5 mm/h. During the sample growth the temperature gradient of � 2.2 K/cm along the am- poule was maintained. When the crystal fully filled the ampoule, the growth process of the sample was terminated and the temperature gradient was reduced to about 1.1 K/cm. Next, the sample was cooled. The cooling rate of the sample was about 0.1 K/h in the temperature range 173–100 K, � 0.2 K/h in the range 100–70 K and � 0.5 K/h below 70 K. At liquid he- lium temperatures the sample was transparent without any visible defects or voids. When the sample was at © V.V. Sumarokov, P. Stachowiak, and A. Je¿owski, 2003 the temperature of � 4.2 K, before the measurements start, gaseous helium at pressure of � 1 kPa was ad- mitted to the ampoule to improve thermal contact of the sample with the two thermometers and the gradi- ent heater. Measurements of the thermal conductivity of CO2 were performed by steady state flow method. The experimental error did not exceed 10%. Other detail of the experiment has been described in Refs. 4–6. Results and discussion The results of the measurements of the thermal con- ductivity coefficient dependence on temperature for solid CO2 in the temperature range 1.5–36 K have been depicted in Fig. 1. In the figure earlier high-tem- perature carbon dioxide data of Koloskova et al. [3] have also been included. In terms of quality, the dependence of the thermal conductivity on temperature, �(T), obtained in the experiment is typical for a dielectric crystal, see, e.g., [1,2]. Initially, in the lowest temperatures, the ther- mal conductivity increases with increasing tempera- ture, then at temperature around 5 K the coefficient attains its maximum value. For temperatures corre- sponding those above the maximum, the thermal con- ductivity initially quickly decreases, following the ex- ponential decay, and then the decrease becomes weaker. The maximum value of the thermal conduc- tivity coefficient � of 720 W/(m�K) should be no- ticed. This value is much greater than any of those for other (so-far investigated) simple molecular crystals [5–8], except the solid para-hydrogen [7] — for com- parison also the data obtained earlier for crystals of pure nitrogen [5], nitrous oxide [7] and para-hydro- gen [8] have been depicted in Fig. 1. Despite high maximum value of the thermal con- ductivity, which can be regarded as an evidence for good quality of the investigated carbon dioxide crystal and high chemical purity of the sample, the depend- ence �(T) in low temperatures is far from typical for low-defect-content dielectric crystal. In the standard case of a dielectric crystal with low density of point defects and dislocations, the low-temperature thermal conductivity is specified by scattering of phonons on grain or sample boundaries, which (being independent from the phonon frequency) give � � T3. In the case of our CO2 sample the dependence is � � T1.7. This de- pendence is close to that observed in case of prevailing scattering of phonons on dislocation strain fields [9]. Assuming predominating in low temperatures scatter- ing of phonons on dislocations in CO2 and using the information on crystal structure obtained from analy- sis of nitrogen thermal conductivity data [5] (where boundary scattering dominated in low temperatures) one can estimate the order of the grain size of the in- vestigated carbon dioxide crystal, as follows. From the thermal conductivity expression for a gas, � � � 1 3 Cvl (where C stands for the specific heat of phonon gas, v for the velocity of propagation of pho- nons and l for the phonon mean free path — in this particular case limited by the sample grains size) one gets the grain size of the CO2 sample �10 mm. The above result has been obtained by assuming specific heat of N2 about ten times greater than that of CO2 [1], the same phonon propagation velocity in nitrogen and in carbon dioxide [1], and by taking (from the ex- periments) the ratio � �CO N2 2 / � 100, and the nitro- gen crystal grain size of the order of � 10–2 mm (from Ref. 5). It means that in our experiment we dealt with a large-grained sample, possibly with a single crystal. High thermal conductivity in higher temperatures may result from relatively low anharmonicity of CO2 molecule translational vibrations and, therefore, weak phonon—phonon interaction. More detailed analysis of the results of measure- ments of the dependence of thermal conductivity on temperature for solid carbon dioxide will be published elsewhere. 604 Fizika Nizkikh Temperatur, 2003, v. 29, No. 5 V.V. Sumarokov, P. Stachowiak, and A. Je¿owski 1 10 100 �T1.7 – our results for CO2 – Koloskova et al.[3] – Data for N2 [5] – Data for N2 2 O [7] – Data for p -H [8] T, K 1 10 10 10 , W /( m K ) � 3 2 Fig. 1. Temperature dependence of thermal conductivity coefficient of solid carbon dioxide. Earlier data for nitro- gen, para-hydrogen and nitrous oxide crystals have also been included. 1. Physics of Cryocrystals, Yu.A. Freiman and V.G. Manzhelii (eds.), AIP, New York (1996). 2. V.G. Manzhelii, A.I. Prochvatilov, V.G. Gavrilko, and A.I. Isakina, Structure and Thermodynamic Pro- perties of Cryocrystals, Begell House, New York (1998). 3. L.A. Koloskova, I.N. Krupskii, V.G. Manzhelii, B.Ya. Gorodilov, and Yu.G. Kravchenko, Fiz. Tverd. Tela 16, 3089 (1974) [Sov. Phys. Solid State 16, 1993 (1974)]; Fiz. Kondens. Sost., Institute for Low Tem- perature Physics and Engeneering (Kharkov), USSR, No. 31 (1974), p. 69. 4. A. Je¿owski and P. Stachowiak, Cryogenics 32, 601 (1992). 5. P. Stachowiak, V.V. Sumarokov, J. Mucha, and A. Je- ¿owski, Phys. Rev. B50, 543 (1994). 6. P. Stachowiak, V.V. Sumarokov, J. Mucha, and A. Je- ¿owski, J. Low Temp. Phys. 111, 379 (1998). 7. P. Stachowiak, V.V. Sumarokov, J. Mucha, and A. Je- ¿owski, The Conference on Cryocrystals and Quatum Crystals, Freising’2002, poster presentation. 8. O.A. Korolyuk, B.Ya. Gorodilov, A.I. Krivchikov, and V.G. Manzhelii, Fiz. Nizk. Temp. 25, 944 (1999) [Low Temp. Phys. 25, 708 (1999)]. 9. R. Berman, Thermal Conduction in Solids, Clarendon, Oxford (1976). Low-temperature thermal conductivity of solid carbon dioxide Fizika Nizkikh Temperatur, 2003, v. 29, No. 5 605