TY - JOUR
T1 - Anomalous temperature behavior of impurities in lead and silver hosts
AU - Newville, Matthew
AU - Stern, E. A.
AU - Haskel, D.
AU - Shechter, H.
AU - Yacoby, Y.
PY - 1993/1
Y1 - 1993/1
N2 - XAFS and Mossbauer effect measurements were made on impurities that lower the bulk melting temperature, Tm, of Pb and Ag. In addition XAFS measurements were made on T1 impurities that raise Tmof Pb. The spectral intensity of the Mossbauer signal in Pb varies as expected from harmonic vibrations of the 1 at.% Sn Mossbauer atoms below a temperature of about 140K. Above this temperature the spectral intensity drops rapidly which is attributed to a localized hopping associated with a high entropy density. In Ag hosts a similar behavior occurs above 900K. The XAFS signal from Hg impurities in Pb, which like Sn lowers Tm, starts deviating from vibrational behavior above 400K where the apparent coordination number decreases. This is also interpreted as a localized hopping. However, Tl, which raises Tm, shows the normal vibrational behavior in XAFS measurements in a Pb host. XAFS measurements on Ga impurities in Ag, which also lower Tm of bulk Ag, show only expected anharmonic behavior up to 900K. All of these results suggest a liquid-like high entropy region within a radius of somewhat more than an atomic spacing around impurities that lower Tm. These high entropy, or “premelted”, regions could act as nucleation sites for three dimensional melting and should dominate over both grain boundaries and free surfaces in nucleating bulk melting in large single crystals.
AB - XAFS and Mossbauer effect measurements were made on impurities that lower the bulk melting temperature, Tm, of Pb and Ag. In addition XAFS measurements were made on T1 impurities that raise Tmof Pb. The spectral intensity of the Mossbauer signal in Pb varies as expected from harmonic vibrations of the 1 at.% Sn Mossbauer atoms below a temperature of about 140K. Above this temperature the spectral intensity drops rapidly which is attributed to a localized hopping associated with a high entropy density. In Ag hosts a similar behavior occurs above 900K. The XAFS signal from Hg impurities in Pb, which like Sn lowers Tm, starts deviating from vibrational behavior above 400K where the apparent coordination number decreases. This is also interpreted as a localized hopping. However, Tl, which raises Tm, shows the normal vibrational behavior in XAFS measurements in a Pb host. XAFS measurements on Ga impurities in Ag, which also lower Tm of bulk Ag, show only expected anharmonic behavior up to 900K. All of these results suggest a liquid-like high entropy region within a radius of somewhat more than an atomic spacing around impurities that lower Tm. These high entropy, or “premelted”, regions could act as nucleation sites for three dimensional melting and should dominate over both grain boundaries and free surfaces in nucleating bulk melting in large single crystals.
KW - Impurities
KW - Mossbauer
KW - Xafs
UR - http://www.scopus.com/inward/record.url?scp=84956086993&partnerID=8YFLogxK
U2 - 10.7567/JJAPS.32S2.628
DO - 10.7567/JJAPS.32S2.628
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AN - SCOPUS:84956086993
SN - 0021-4922
VL - 32
SP - 628
EP - 630
JO - Japanese Journal of Applied Physics
JF - Japanese Journal of Applied Physics
ER -