TY - JOUR
T1 - High Hole Mobility and Nonsaturating Giant Magnetoresistance in the New 2D Metal NaCu4Se4 Synthesized by a Unique Pathway
AU - Chen, Haijie
AU - Rodrigues, Joao N.B.
AU - Rettie, Alexander J.E.
AU - Song, Tze Bin
AU - Chica, Daniel G.
AU - Su, Xianli
AU - Bao, Jin Ke
AU - Chung, Duck Young
AU - Kwok, Wai Kwong
AU - Wagner, Lucas K.
AU - Kanatzidis, Mercouri G.
N1 - Funding Information:
Research at Argonne primarily was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Computational resources utilized in first-principles calculations were provided by the University of Illinois Campus Cluster and the Center for Advanced 2D Materials Cluster in Singapore. SEM-EDS work was performed by use of the EPIC, Keck-II, and/or SPID facility(ies) of Northwestern University’s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSF DMR-1121262) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN.
Publisher Copyright:
© 2018 American Chemical Society.
PY - 2019/1/9
Y1 - 2019/1/9
N2 - The new compound NaCu 4 Se 4 forms by the reaction of CuO and Cu in a molten sodium polyselenide flux, with the existence of CuO being unexpectedly critical to its synthesis. It adopts a layered hexagonal structure (space group P6 3 /mmc with cell parameters a = 3.9931(6) Å and c = 25.167(5) Å), consisting of infinite two-dimensional [Cu 4 Se 4 ] - slabs separated by Na + cations. X-ray photoelectron spectroscopy suggests that NaCu 4 Se 4 is mixed-valent with the formula (Na + )(Cu + ) 4 (Se 2- )(Se - )(Se 2 ) 2- . NaCu 4 Se 4 is a p-type metal with a carrier density of â10 21 cm -3 and a high hole mobility of â808 cm 2 V -1 s -1 at 2 K based on electronic transport measurements. First-principles calculations suggest the density of states around the Fermi level are composed of Cu-d and Se-p orbitals. At 2 K, a very large transverse magnetoresistance of â1400% was observed, with a nonsaturating, linear dependence on field up to 9 T. Our results indicate that the use of metal oxide chemical precursors can open reaction paths to new low-dimensional compounds.
AB - The new compound NaCu 4 Se 4 forms by the reaction of CuO and Cu in a molten sodium polyselenide flux, with the existence of CuO being unexpectedly critical to its synthesis. It adopts a layered hexagonal structure (space group P6 3 /mmc with cell parameters a = 3.9931(6) Å and c = 25.167(5) Å), consisting of infinite two-dimensional [Cu 4 Se 4 ] - slabs separated by Na + cations. X-ray photoelectron spectroscopy suggests that NaCu 4 Se 4 is mixed-valent with the formula (Na + )(Cu + ) 4 (Se 2- )(Se - )(Se 2 ) 2- . NaCu 4 Se 4 is a p-type metal with a carrier density of â10 21 cm -3 and a high hole mobility of â808 cm 2 V -1 s -1 at 2 K based on electronic transport measurements. First-principles calculations suggest the density of states around the Fermi level are composed of Cu-d and Se-p orbitals. At 2 K, a very large transverse magnetoresistance of â1400% was observed, with a nonsaturating, linear dependence on field up to 9 T. Our results indicate that the use of metal oxide chemical precursors can open reaction paths to new low-dimensional compounds.
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U2 - 10.1021/jacs.8b11911
DO - 10.1021/jacs.8b11911
M3 - Article
C2 - 30537833
AN - SCOPUS:85059869532
SN - 0002-7863
VL - 141
SP - 635
EP - 642
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 1
ER -