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A thermodynamic explanation of the Invar effect

Journal Article · · Nature Physics
 [1];  [2];  [3];  [3];  [3];  [4];  [5];  [2];  [3]
  1. California Institute of Technology (CalTech), Pasadena, CA (United States); Boston College
  2. Boston College, Chestnut Hill, MA (United States)
  3. California Institute of Technology (CalTech), Pasadena, CA (United States)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  5. Weizmann Institute of Science, Rehovot (Israel)
+ Show Author Affiliations
The anomalously low thermal expansion of Fe–Ni Invar has long been associated with magnetism, but to date, the microscopic underpinnings of the Invar behaviour have eluded both theory and experiment. Here we present nuclear resonant X-ray scattering measurements of the phonon and magnetic entropies under pressure. By applying a thermodynamic Maxwell relation to these data, we obtain the separate phonon and magnetic contributions to thermal expansion. We find that the Invar behaviour stems from a competition between phonons and spins. In particular, the phonon contribution to thermal expansion cancels the magnetic contribution over the 0–3 GPa pressure range of Invar behaviour. At pressures above 3 GPa, the cancellation is lost, but our analysis reproduces the positive thermal expansion measured separately by synchrotron X-ray diffractometry. Ab initio calculations informed by experimental data show that spin–phonon interactions improve the accuracy of this cancellation over the range of Invar behaviour. Further, spin–phonon interactions also explain how different phonon modes have different energy shifts with pressure.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Boston College, Chestnut Hill, MA (United States); University of Illinois, Chicago, IL (United States)
Sponsoring Organization:
National Science Foundation (NSF); Swedish Research Council (VR); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357; FG02-94ER14466; NA0003975; SC0021071
OSTI ID:
1993279
Alternate ID(s):
OSTI ID: 2429448
OSTI ID: 2205672
Journal Information:
Nature Physics, Journal Name: Nature Physics Journal Issue: 11 Vol. 19; ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)Copyright Statement
Country of Publication:
United States
Language:
English

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