X-ray diffraction and equation of state of the C–S–H room-temperature superconductor

Lamichhane, Anmol; Kumar, Ravhi; Ahart, Muhtar; Salke, Nilesh P.; Dasenbrock-Gammon, Nathan; Snider, Elliot; Meng, Yue; Lavina, Barbara; Chariton, Stella; Prakapenka, Vitali B.; Somayazulu, Maddury; Dias, Ranga P.; Hemley, Russell J.

doi:10.1063/5.0064750

Title: X-ray diffraction and equation of state of the C–S–H room-temperature superconductor

Abstract

X-ray diffraction indicates that the structure of the recently discovered carbonaceous sulfur hydride (C–S–H) room-temperature superconductor is derived from previously established van der Waals compounds found in the H₂S–H₂ and CH₄–H₂ systems. Crystals of the superconducting phase were produced by a photochemical synthesis technique, leading to the superconducting critical temperature T_c of 288 K at 267 GPa. X-ray diffraction patterns measured from 124 to 178 GPa, within the pressure range of the superconducting phase, are consistent with an orthorhombic structure derived from the Al₂Cu-type determined for (H₂S)₂H₂ and (CH₄)₂H₂ that differs from those predicted and observed for the S–H system at these pressures. The formation and stability of the C–S–H compound can be understood in terms of the close similarity in effective volumes of the H₂S and CH₄ components, and denser carbon-bearing S–H phases may form at higher pressures. Furthermore, the results are crucial for understanding the very high superconducting T_c found in the C–S–H system at megabar pressures.

Authors:

^[1]; Kumar, Ravhi ^[1];

^[1]; Salke, Nilesh P. ^[1];

^[2];

^[2]; Meng, Yue ^[3]; Lavina, Barbara ^[4];

^[1]; Prakapenka, Vitali B. ^[1]; Somayazulu, Maddury ^[3];

^[2];

^[1]

Univ. of Illinois, Chicago, IL (United States)
Univ. of Rochester, NY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Publication Date:: Tue Sep 21 00:00:00 EDT 2021

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Illinois, Chicago, IL (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Fusion Energy Sciences (FES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF); Chicago/DOE Alliance Center (CDAC)

OSTI Identifier:: 1839908

Alternate Identifier(s):: OSTI ID: 1821225

Grant/Contract Number:: AC02-06CH11357; NA0003975; SC0020340; DMR-1933622; DMR-1809649; EAR-1634415

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 155; Journal Issue: 11; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; diamond anvil cells; superconductivity; doping; superconductors; x-ray diffraction; phase transitions; raman spectroscopy; equations of state; perovskites

Citation Formats


                    Lamichhane, Anmol, Kumar, Ravhi, Ahart, Muhtar, Salke, Nilesh P., Dasenbrock-Gammon, Nathan, Snider, Elliot, Meng, Yue, Lavina, Barbara, Chariton, Stella, Prakapenka, Vitali B., Somayazulu, Maddury, Dias, Ranga P., and Hemley, Russell J. X-ray diffraction and equation of state of the C–S–H room-temperature superconductor.  United States: N. p., 2021. 
Web.  doi:10.1063/5.0064750.

Copy to clipboard


                    Lamichhane, Anmol, Kumar, Ravhi, Ahart, Muhtar, Salke, Nilesh P., Dasenbrock-Gammon, Nathan, Snider, Elliot, Meng, Yue, Lavina, Barbara, Chariton, Stella, Prakapenka, Vitali B., Somayazulu, Maddury, Dias, Ranga P., & Hemley, Russell J. X-ray diffraction and equation of state of the C–S–H room-temperature superconductor.  United States.  https://doi.org/10.1063/5.0064750

Copy to clipboard


                    Lamichhane, Anmol, Kumar, Ravhi, Ahart, Muhtar, Salke, Nilesh P., Dasenbrock-Gammon, Nathan, Snider, Elliot, Meng, Yue, Lavina, Barbara, Chariton, Stella, Prakapenka, Vitali B., Somayazulu, Maddury, Dias, Ranga P., and Hemley, Russell J. Tue .  
"X-ray diffraction and equation of state of the C–S–H room-temperature superconductor".  United States.  https://doi.org/10.1063/5.0064750.  https://www.osti.gov/servlets/purl/1839908.

Copy to clipboard


                    
@article{osti_1839908,

  title        = {X-ray diffraction and equation of state of the C–S–H room-temperature superconductor},

  author       = {Lamichhane, Anmol and Kumar, Ravhi and Ahart, Muhtar and Salke, Nilesh P. and Dasenbrock-Gammon, Nathan and Snider, Elliot and Meng, Yue and Lavina, Barbara and Chariton, Stella and Prakapenka, Vitali B. and Somayazulu, Maddury and Dias, Ranga P. and Hemley, Russell J.},

  abstractNote = {X-ray diffraction indicates that the structure of the recently discovered carbonaceous sulfur hydride (C–S–H) room-temperature superconductor is derived from previously established van der Waals compounds found in the H2S–H2 and CH4–H2 systems. Crystals of the superconducting phase were produced by a photochemical synthesis technique, leading to the superconducting critical temperature Tc of 288 K at 267 GPa. X-ray diffraction patterns measured from 124 to 178 GPa, within the pressure range of the superconducting phase, are consistent with an orthorhombic structure derived from the Al2Cu-type determined for (H2S)2H2 and (CH4)2H2 that differs from those predicted and observed for the S–H system at these pressures. The formation and stability of the C–S–H compound can be understood in terms of the close similarity in effective volumes of the H2S and CH4 components, and denser carbon-bearing S–H phases may form at higher pressures. Furthermore, the results are crucial for understanding the very high superconducting Tc found in the C–S–H system at megabar pressures.},

  doi          = {10.1063/5.0064750},

  journal      = {Journal of Chemical Physics},

  number       = 11,

  volume       = 155,

  place        = {United States},

  year         = {Tue Sep 21 00:00:00 EDT 2021},

  month        = {Tue Sep 21 00:00:00 EDT 2021}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1063/5.0064750

Other availability

Search WorldCat to find libraries that may hold this journal

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

High-Pressure Compounds in Methane-Hydrogen Mixtures
journal, March 1996

Somayazulu, M. S.; Finger, L. W.; Hemley, R. J.
Science, Vol. 271, Issue 5254, p. 1400-1402
DOI: 10.1126/science.271.5254.1400

Dissociation of methane under high pressure
journal, October 2010

Gao, Guoying; Oganov, Artem R.; Ma, Yanming
The Journal of Chemical Physics, Vol. 133, Issue 14
DOI: 10.1063/1.3488102

Room-temperature superconductivity in a carbonaceous sulfur hydride
journal, October 2020

Snider, Elliot; Dasenbrock-Gammon, Nathan; McBride, Raymond
Nature, Vol. 586, Issue 7829
DOI: 10.1038/s41586-020-2801-z

Properties of diamond under hydrostatic pressures up to 140 GPa
journal, February 2003

Occelli, Florent; Loubeyre, Paul; LeToullec, René
Nature Materials, Vol. 2, Issue 3
DOI: 10.1038/nmat831

X-ray diffraction and equation of state of hydrogen at megabar pressures
journal, October 1996

Loubeyre, P.; LeToullec, R.; Hausermann, D.
Nature, Vol. 383, Issue 6602
DOI: 10.1038/383702a0

X-ray diffraction studies and equation of state of methane at 202GPa
journal, April 2009

Sun, Liling; Yi, Wei; Wang, Lin
Chemical Physics Letters, Vol. 473, Issue 1-3
DOI: 10.1016/j.cplett.2009.03.072

The pressure-temperature phase and transformation diagram for carbon; updated through 1994
journal, January 1996

Bundy, F. P.; Bassett, W. A.; Weathers, M. S.
Carbon, Vol. 34, Issue 2
DOI: 10.1016/0008-6223(96)00170-4

The metallization and superconductivity of dense hydrogen sulfide
journal, May 2014

Li, Yinwei; Hao, Jian; Liu, Hanyu
The Journal of Chemical Physics, Vol. 140, Issue 17
DOI: 10.1063/1.4874158

Bonding Changes in Compressed Superhard Graphite
journal, October 2003

Mao, W. L.
Science, Vol. 302, Issue 5644
DOI: 10.1126/science.1089713

Hole-doped room-temperature superconductivity in H3S1-xZ (Z=C, Si)
journal, December 2020

Ge, Yanfeng; Zhang, Fan; Dias, Ranga P.
Materials Today Physics, Vol. 15
DOI: 10.1016/j.mtphys.2020.100330

Pressure-induced superconducting ternary hydride H3SXe: A theoretical investigation
journal, August 2018

Li, Da; Liu, Yan; Tian, Fu-Bo
Frontiers of Physics, Vol. 13, Issue 5
DOI: 10.1007/s11467-018-0818-7

Structure and compression of crystalline methane at high pressure and room temperature
journal, August 1980

Hazen, R. M.; Mao, H. K.; Finger, L. W.
Applied Physics Letters, Vol. 37, Issue 3
DOI: 10.1063/1.91909

Potential high- T _c superconducting lanthanum and yttrium hydrides at high pressure
journal, June 2017

Liu, Hanyu; Naumov, Ivan I.; Hoffmann, Roald
Proceedings of the National Academy of Sciences, Vol. 114, Issue 27
DOI: 10.1073/pnas.1704505114

Superconductivity at 250 K in lanthanum hydride under high pressures
journal, May 2019

Drozdov, A. P.; Kong, P. P.; Minkov, V. S.
Nature, Vol. 569, Issue 7757
DOI: 10.1038/s41586-019-1201-8

Crystal structure of graphite under room-temperature compression and decompression
journal, July 2012

Wang, Yuejian; Panzik, Joseph E.; Kiefer, Boris
Scientific Reports, Vol. 2, Issue 1
DOI: 10.1038/srep00520

Anomalous High‐Temperature Superconductivity in YH ₆
journal, March 2021

Troyan, Ivan A.; Semenok, Dmitrii V.; Kvashnin, Alexander G.
Advanced Materials, Vol. 33, Issue 15
DOI: 10.1002/adma.202006832

Pressure-induced metallization of dense (H2S)2H2 with high-Tc superconductivity
journal, November 2014

Duan, Defang; Liu, Yunxian; Tian, Fubo
Scientific Reports, Vol. 4, Issue 1
DOI: 10.1038/srep06968

Conventional superconductivity at 203 kelvin at high pressures in the sulfur hydride system
journal, August 2015

Drozdov, A. P.; Eremets, M. I.; Troyan, I. A.
Nature, Vol. 525, Issue 7567
DOI: 10.1038/nature14964

DIOPTAS : a program for reduction of two-dimensional X-ray diffraction data and data exploration
journal, May 2015

Prescher, Clemens; Prakapenka, Vitali B.
High Pressure Research, Vol. 35, Issue 3
DOI: 10.1080/08957959.2015.1059835

Evidence for Superconductivity above 260 K in Lanthanum Superhydride at Megabar Pressures
journal, January 2019

Somayazulu, Maddury; Ahart, Muhtar; Mishra, Ajay K.
Physical Review Letters, Vol. 122, Issue 2
DOI: 10.1103/PhysRevLett.122.027001

Superconductivity up to 243 K in the yttrium-hydrogen system under high pressure
journal, August 2021

Kong, Panpan; Minkov, Vasily S.; Kuzovnikov, Mikhail A.
Nature Communications, Vol. 12, Issue 1
DOI: 10.1038/s41467-021-25372-2

Crystal structure of the superconducting phase of sulfur hydride
journal, May 2016

Einaga, Mari; Sakata, Masafumi; Ishikawa, Takahiro
Nature Physics, Vol. 12, Issue 9
DOI: 10.1038/nphys3760

Superconductivity at 100 K in dense SiH4(H2)2 predicted by first principles
journal, August 2010

Li, Y.; Gao, G.; Xie, Y.
Proceedings of the National Academy of Sciences, Vol. 107, Issue 36
DOI: 10.1073/pnas.1007354107

Similar Records in DOE PAGES and OSTI.GOV collections:

Hole-doped room-temperature superconductivity in H₃S_1-xZ (Z=C, Si)

Journal Article Ge, Yanfeng ; Zhang, Fan ; Dias, Ranga P. ; ... - Materials Today Physics

We examine the effects of the low-level substitution of S atoms by C and Si atoms on the superconductivity of H₃S with the Im3¯m structure at megabar pressures. The hole doping can fine-tune the Fermi energy to reach the electronic density-of-states peak maximizing the electron-phonon coupling. This can boost the critical temperature from the original 203 K to 289 K and 283 K, respectively, for H₃S_0.962C_0.038 at 260 GPa and H₃S_0.960Si_0.040 at 230 GPa. The former may provide an explanation for the recent experimental observation of room-temperature superconductivity in a highly compressed CeSeH system. Our work opens a new avenuemore »« less
https://doi.org/10.1016/j.mtphys.2020.100330

Full Text Available
Room-temperature superconductivity in boron- and nitrogen-doped lanthanum superhydride

Journal Article Ge, Yanfeng ; Zhang, Fan ; Hemley, Russell J. - Physical Review. B

Recent theoretical and experimental studies of hydrogen-rich materials at megabar pressures (i.e., >100 GPa) have led to the discovery of very high-temperature superconductivity in these materials. Lanthanum superhydride LaH10 has been of particular focus as the first material to exhibit a superconducting critical temperature (T_c) near room temperature. Experiments indicate that the use of ammonia borane as the hydrogen source can increase the conductivity onset temperatures of lanthanum superhydride to as high as 290 K. In this work, we examine the doping effects of B and N atoms on the superconductivity of LaH₁₀ in its fcc (more »« less
https://doi.org/10.1103/physrevb.104.214505

Full Text Available
Synthesis and structure of carbon-doped H₃S compounds at high pressure

Journal Article Goncharov, Alexander F. ; Bykova, Elena ; Bykov, Maxim ; ... - Journal of Applied Physics

Understanding of recently reported putative close-to-room-temperature superconductivity in C-S-H compounds at 267 GPa demands a reproducible synthesis protocol as well as knowledge of the compounds' structure and composition. Here, we synthesized C-S-H compounds with various carbon compositions at high pressures from elemental carbon C and methane CH₄, sulfur S, and molecular hydrogen H₂. Here, we focus on compounds synthesized using methane as these allow a straightforward determination of their structure and composition by combining single-crystal x-ray diffraction and Raman spectroscopy. We applied a two-stage synthesis of [(CH₄)_x(H₂S)_(1-x)]₂H₂ compounds with various compositions by first reacting sulfur and mixed methane-hydrogen fluids and forming CH₄-doped H₂S crystals at 0.5-3 GPa and then by growing single crystals of the desired hydrogen-rich compound. Raman spectroscopy applied to this material shows the presence of CH₄ molecules incorporated into the lattice and allows the determination of the CH₄ content, while single-crystal x-ray diffraction results suggest that the methane molecules substitute H₂S molecules. The structural behavior of these compounds is very similar to the previously investigated methane-free crystals demonstrating a transition from Al₂Cu type I4/mcm molecular crystal to a modulated molecular structure at 20-30 GPa and back to the same basic I4/mcm structure in an extended modification with greatly modified Raman spectra. This latter phase demonstrates a distortion into a Pnma structure at 132-159 GPa and then transforms into a common Immore »« less
https://doi.org/10.1063/5.0073499

Full Text Available
Creating superconductivity in WB₂ through pressure-induced metastable planar defects

Journal Article Lim, J. ; Hire, A. C. ; Quan, Y. ; ... - Nature Communications

High-pressure electrical resistivity measurements reveal that the mechanical deformation of ultra-hard WB₂ during compression induces superconductivity above 50 GPa with a maximum superconducting critical temperature, T_c of 17 K at 91 GPa. Upon further compression up to 187 GPa, the T_c gradually decreases. Theoretical calculations show that electron-phonon mediated superconductivity originates from the formation of metastable stacking faults and twin boundaries that exhibit a local structure resembling MgB₂ (hP3, space group 191, prototype AlB₂). Synchrotron x-ray diffraction measurements up to 145 GPa show that the ambient pressure hP12 structure (space group 194, prototype WB₂) continues to persist to this pressure,more »« less
https://doi.org/10.1038/s41467-022-35191-8

Full Text Available
Room-temperature superconductivity in a carbonaceous sulfur hydride

Journal Article Snider, Elliot ; Dasenbrock-Gammon, Nathan ; McBride, Raymond ; ... - Nature (London)

One of the long-standing challenges in experimental physics is the observation of room-temperature superconductivity (RTSC). Recently, high temperature conventional superconductivity in hydrogen-rich materials has been reported in several systems under high pressure. The most significant discovery in reaching RTSC is the pressure-driven disproportionation of hydrogen sulfide (H₂S) to H₃S with a confirmed Tc of 203 kelvin at 155 gigapascals. As H₂S readily mixes with hydrogen to form guest-host structures at lower pressures, the comparable size of methane to H₂S should allow molecular exchange within a large assemblage of van der Waals solids that are (highly) hydrogen-rich with H₂ inclusions thatmore »« less
https://doi.org/10.1038/s41586-020-2801-z

Full Text Available

Similar Records

Title: X-ray diffraction and equation of state of the C–S–H room-temperature superconductor

Abstract

Citation Formats

High-Pressure Compounds in Methane-Hydrogen Mixtures journal, March 1996

Dissociation of methane under high pressure journal, October 2010

Room-temperature superconductivity in a carbonaceous sulfur hydride journal, October 2020

Properties of diamond under hydrostatic pressures up to 140 GPa journal, February 2003

X-ray diffraction and equation of state of hydrogen at megabar pressures journal, October 1996

X-ray diffraction studies and equation of state of methane at 202GPa journal, April 2009

The pressure-temperature phase and transformation diagram for carbon; updated through 1994 journal, January 1996

The metallization and superconductivity of dense hydrogen sulfide journal, May 2014

Bonding Changes in Compressed Superhard Graphite journal, October 2003

Hole-doped room-temperature superconductivity in H3S1-xZ (Z=C, Si) journal, December 2020

Pressure-induced superconducting ternary hydride H3SXe: A theoretical investigation journal, August 2018

Structure and compression of crystalline methane at high pressure and room temperature journal, August 1980

Potential high- T c superconducting lanthanum and yttrium hydrides at high pressure journal, June 2017

Superconductivity at 250 K in lanthanum hydride under high pressures journal, May 2019

Crystal structure of graphite under room-temperature compression and decompression journal, July 2012

Anomalous High‐Temperature Superconductivity in YH 6 journal, March 2021

Pressure-induced metallization of dense (H2S)2H2 with high-Tc superconductivity journal, November 2014

Conventional superconductivity at 203 kelvin at high pressures in the sulfur hydride system journal, August 2015

DIOPTAS : a program for reduction of two-dimensional X-ray diffraction data and data exploration journal, May 2015

Evidence for Superconductivity above 260 K in Lanthanum Superhydride at Megabar Pressures journal, January 2019

Superconductivity up to 243 K in the yttrium-hydrogen system under high pressure journal, August 2021

Crystal structure of the superconducting phase of sulfur hydride journal, May 2016

Superconductivity at 100 K in dense SiH4(H2)2 predicted by first principles journal, August 2010

High-Pressure Compounds in Methane-Hydrogen Mixtures
journal, March 1996

Dissociation of methane under high pressure
journal, October 2010

Room-temperature superconductivity in a carbonaceous sulfur hydride
journal, October 2020

Properties of diamond under hydrostatic pressures up to 140 GPa
journal, February 2003

X-ray diffraction and equation of state of hydrogen at megabar pressures
journal, October 1996

X-ray diffraction studies and equation of state of methane at 202GPa
journal, April 2009

The pressure-temperature phase and transformation diagram for carbon; updated through 1994
journal, January 1996

The metallization and superconductivity of dense hydrogen sulfide
journal, May 2014

Bonding Changes in Compressed Superhard Graphite
journal, October 2003

Hole-doped room-temperature superconductivity in H3S1-xZ (Z=C, Si)
journal, December 2020

Pressure-induced superconducting ternary hydride H3SXe: A theoretical investigation
journal, August 2018

Structure and compression of crystalline methane at high pressure and room temperature
journal, August 1980

Potential high- T _c superconducting lanthanum and yttrium hydrides at high pressure
journal, June 2017

Superconductivity at 250 K in lanthanum hydride under high pressures
journal, May 2019

Crystal structure of graphite under room-temperature compression and decompression
journal, July 2012

Anomalous High‐Temperature Superconductivity in YH ₆
journal, March 2021

Pressure-induced metallization of dense (H2S)2H2 with high-Tc superconductivity
journal, November 2014

Conventional superconductivity at 203 kelvin at high pressures in the sulfur hydride system
journal, August 2015

DIOPTAS : a program for reduction of two-dimensional X-ray diffraction data and data exploration
journal, May 2015

Evidence for Superconductivity above 260 K in Lanthanum Superhydride at Megabar Pressures
journal, January 2019

Superconductivity up to 243 K in the yttrium-hydrogen system under high pressure
journal, August 2021

Crystal structure of the superconducting phase of sulfur hydride
journal, May 2016

Superconductivity at 100 K in dense SiH4(H2)2 predicted by first principles
journal, August 2010