1
Reference TBTDEN 1. Background Development of NbN films by atomic layer deposition for Superconducting Tunnel Junction particle detectors with a high operating temperature M. Ukibe, and Go Fujii National Institute of Advanced Industrial Science and Technology, 1-1-1, Umezono, Tsukuba, Ibaraki, 305-8568, JAPAN Nanoelectronics Research Center A) Understanding the evolution of molecules in space need to evaluate quantitatively dissociation branching ratios and the yields of neutral products in dissociative electron-ion recombination (DR) processes. The combination of a solid-state kinetic-energy-sensitive superconducting tunnel junction (STJ) particle detector and tandem mass spectrometers (MS) or a compact electrostatic storage rings.[2][3] [2] M. Ohkubo, et al., IJMS 299, 94 (2011), doi: 10.1016/j.ijms.2010.09.027 B) The powerful analytical instrument of the DR processes fabricated at AIST MS/KEMS instrument, AIST, Tsukuba Lab-based MS/MS [3] T. Tanabe, et. al., Dissociative Recombination of Molecular Ions with Electrons, p.p. 75-85(2003) [1] Scott Sandford, et. al., The Astronomy and Astrophysics Decadal Survey, Science White Papers,257(2009) [1] Solid state kinetic-energy-sensitive Nb/Al STJ detector Electrostatic Storage Ring or MS instruments + 2. Difficulties of the STJ operation in MS A) An appropriate operation temperature of Nb/Al STJs : 0.3 K IR shield Particles can pass through holes in IR shield B) Large thermal inflows from room temperature to STJs for a high throughput A large number of wirings (>100) for obtaining a large detection area Insufficient thermal filter setup for the particles sources It is necessary for particles to pass IR shields C) STJ detectors with high operation temperature > 1 K Operation temperature < Transition temperature (T C ) / 10 NbN (T C : 17.8 K for 100 nm[4] ) is appropriate [4] A. Shoji, IEEE Tran. Mag. 27, p.p. 3184(1991) D) NbN/AlN/NbN STJ (NbN-STJ) Nice lattice matching : NbN(0.439 nm (a-axis)) and AlN (0.498 nm (c-axis)) Full nitride multilayer AlN thickness should be controlled between 1.4 and 1.6 nm in order to realize a J C value between 100 and 1000 A/cm 2 [5] [5] Z. Wang, et. Al., Appl. Phys. Lett., 75, p.p. 701(1999) Full epitaxial multilayer Good tunnel barrier E) Atomic layer deposition (ALD) is best for the deposition of NbN-STJs NbN films deposited by an ALD tended to exhibit a low T C of about 10 K [6]. 3. Experiments [6] Mario Ziegler et.al., Supercond. Sci. Technol. 26, 025008 (2013) • Source (precursors) of NbN : TBTDEN [C 16 H 39 N 4 Nb] • Substrate : M-plain sapphire wafer • ALD : Ultratech Fiji 200 G2 • Substrate temperature(T sub ) : 570 K • Film thickness (t NbN ) : 50 nm • Dissociation of TBTDEN : N 2 plasma [7] http://www.longsun.asia/uploadfile/upload/2015072113420828.pdf Ultratech Fiji 200 G2 [7] A) Deposition condition We have tried improving the superconducting properties of ALD NbN films by a post-deposition RTP to realize a high T C about 17 K. B) Anneal condition • Annealer : ANNEALSYS AS-One 100 • Process gas : N 2 at of 1 atm • Anneal temperature : 770, 870, 970, 1050, 1120 K • Temperature ramp rate : 50 K/sec • Anneal time : 20 ~ 2000 sec AS-One 100 C) Evaluation of film characteristics (i) X-ray diffraction Diffractometer :Rigaku Ultima X Multipurpose X-ray diffraction system Measurement : Grazing incident(0.6 degree), θ-2θ, In-plane, φ-scan, Pole figure (ii) Surface morphology • SPM : Shimadzu SFT-4500 scanning probe microscope • Scan area : 500 x 500 nm (iii) R-T curve Pattern size : A line patter of 50 µm width and 1 mm long Cryostat : 4K GM 4. Results X-ray diffraction pattern(GI) of a NbN film annealed at 870 K, 200 sec. A) Crystal structure ALD NbN film on M-plain sapphire wafer : 110 orientation After the anneal process at 970 K, a part of the cubic NbN transformed into tetragonal NbN. Crystallite size : ALD film(9-11 nm) < Sputter film (14-16 nm) Best crystallinity so far at 870 K, 200 sec Pole figure of a NbN film annealed at 770 K, 2000 sec. It shows that the NbN film has 110 orientation. B) Surface morphology The surface of the NbN film became rough by the anneal. With increasing the anneal temperature, the root mean square roughness (S q ) was considerably enlarged but wasn’t larger than that of the sputter film. The grain size of the NbN in the ALD film increased by the anneal too. C) R-T curves The TC of the ALD NbN film was 12.35 K, higher than that of the previous data [6] and was increased to 13.37K by the anneal of 770K, 2000 sec. The RRR values of the ALD NbN films were smaller than that of the sputter film. 5. Conclusion We succeeded in depositing a 50 nm - thick NbN film on M-plain sapphire with relatively high T C of 12.35 K. The anneal certainly changed the crystal structure conditions of the ALD NbN films and the T C was improved up to 13.37 K. It is considered that the enlargement of the grain size of the NbN by the anneal process was occurred by an agglutination of many NbN crystallites, not by the crystal growth of each NbN crystallite. It is necessary to perform the further investigation in order to decide the optimal anneal condition of the ALD NbN films. This work was supported by JSPS KAKENHI Grant Number 15H03599. A part of this work was conducted at the AIST Nano-Processing Facility. Acknowledgment The authors thank H. Yamamori and S. Shiki for their help with the experiments, and the clean room members of analog-digital superconductivity (CRAVITY) for performing experiments. 6-16am-Poster-2 Peak intensity (cps) δ-NbN(111) δ-NbN(200) δ-NbN(220) β-Nb 2 N(103) δ-NbN(311) δ-NbN(222) δ-NbN(400) γ-NbN(110) 101 011 110 1-10 -110 10-1 01-1 2 1 1 2 2 2 3 3 3 3 0.00E+00 5.00E+02 1.00E+03 1.50E+03 2.00E+03 2.50E+03 3.00E+03 13.00 13.20 13.40 13.60 13.80 14.00 Resistivity (ohm) Temperature (K)

6-16am-Poster-2 Nanoelectronics Research Center ... session...6-16am-Poster-2 Peak intensity (cps) δ-NbN (111) δ-NbN (200) δ-NbN (220) β-Nb 2 N(103) δ-NbN (311) δ-NbN (222) δ-NbN

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  • Reference

    TBTDEN

    1. Background

    Development of NbN films by atomic layer deposition for Superconducting Tunnel Junction particle detectors with a high

    operating temperatureM. Ukibe, and Go Fujii

    National Institute of Advanced Industrial Science and Technology, 1-1-1, Umezono, Tsukuba, Ibaraki, 305-8568, JAPAN

    Nanoelectronics Research Center

    A) Understanding the evolution of molecules in spaceneed to evaluate quantitatively dissociationbranching ratios and the yields of neutral products indissociative electron-ion recombination (DR)processes.

    The combination of a solid-state kinetic-energy-sensitive superconductingtunnel junction (STJ) particle detector and tandem mass spectrometers (MS) ora compact electrostatic storage rings.[2][3]

    [2] M. Ohkubo, et al., IJMS 299, 94 (2011), doi: 10.1016/j.ijms.2010.09.027

    B) The powerful analytical instrument of the DR processes

    fabricated at AISTMS/KEMS instrument, AIST, Tsukuba

    Lab-based MS/MS

    [3] T. Tanabe, et. al., Dissociative Recombination of Molecular Ions with Electrons, p.p. 75-85(2003)

    [1] Scott Sandford, et. al., The Astronomy and Astrophysics Decadal Survey, Science White Papers,257(2009)

    [1]

    Solid state kinetic-energy-sensitive

    Nb/Al STJ detector Electrostatic Storage Ring

    or

    MS instruments

    +

    2. Difficulties of the STJ operation in MSA) An appropriate operation temperature of Nb/Al STJs : 0.3 K

    IR shield

    Particles can pass through holes in IR shield

    B) Large thermal inflows from room temperature to STJs for a high throughputA large number of wirings (>100) for obtaining a large detection areaInsufficient thermal filter setup for the particles sources

    It is necessary for particles to pass IR shieldsC) STJ detectors with high operation temperature > 1 K

    Operation temperature < Transition temperature (TC ) / 10NbN (TC : 17.8 K for 100 nm[4] ) is appropriate

    [4] A. Shoji, IEEE Tran. Mag. 27, p.p. 3184(1991)

    D) NbN/AlN/NbN STJ (NbN-STJ)Nice lattice matching : NbN(0.439 nm (a-axis)) and AlN (0.498 nm (c-axis))

    Full nitride multilayerAlN thickness should be controlled between 1.4 and 1.6 nm in order to realize a JC value between 100 and 1000 A/cm2[5]

    [5] Z. Wang, et. Al., Appl. Phys. Lett., 75, p.p. 701(1999)

    Full epitaxial multilayerGood tunnel barrier

    E) Atomic layer deposition (ALD) is best for the deposition of NbN-STJsNbN films deposited by an ALD tended to exhibit a low TC of about 10 K [6].

    3. Experiments

    [6] Mario Ziegler et.al., Supercond. Sci. Technol. 26, 025008 (2013)

    • Source (precursors) of NbN : TBTDEN [C16H39N4Nb]• Substrate : M-plain sapphire wafer• ALD : Ultratech Fiji 200 G2 • Substrate temperature(Tsub) : 570 K• Film thickness (tNbN) : 50 nm• Dissociation of TBTDEN : N2 plasma

    [7] http://www.longsun.asia/uploadfile/upload/2015072113420828.pdf

    Ultratech Fiji 200 G2 [7]

    A) Deposition condition

    We have tried improving the superconducting properties of ALD NbNfilms by a post-deposition RTP to realize a high TC about 17 K.

    B) Anneal condition• Annealer : ANNEALSYS AS-One 100• Process gas : N2 at of 1 atm• Anneal temperature : 770, 870, 970, 1050, 1120 K• Temperature ramp rate : 50 K/sec • Anneal time : 20 ~ 2000 sec

    AS-One 100

    C) Evaluation of film characteristics(i) X-ray diffraction • Diffractometer :Rigaku Ultima X Multipurpose X-ray diffraction system• Measurement : Grazing incident(0.6 degree), θ-2θ, In-plane, φ-scan, Pole figure (ii) Surface morphology• SPM : Shimadzu SFT-4500 scanning probe microscope• Scan area : 500 x 500 nm(iii) R-T curve• Pattern size : A line patter of 50 µm width and 1 mm long• Cryostat : 4K GM

    4. Results

    X-ray diffraction pattern(GI) of a NbN film annealedat 870 K, 200 sec.

    A) Crystal structure• ALD NbN film on M-plain sapphire wafer : 110 orientation• After the anneal process at 970 K, a part of the cubic NbN transformed into

    tetragonal NbN.• Crystallite size : ALD film(9-11 nm) < Sputter film (14-16 nm)• Best crystallinity so far at 870 K, 200 sec

    Pole figure of a NbN film annealed at 770 K, 2000 sec. Itshows that the NbN film has 110 orientation.

    B) Surface morphology• The surface of the NbN film became rough by the anneal.• With increasing the anneal temperature, the root mean square roughness (Sq)

    was considerably enlarged but wasn’t larger than that of the sputter film.• The grain size of the NbN in the ALD film increased by the anneal too.

    C) R-T curves• The TC of the ALD NbN film was 12.35 K,

    higher than that of the previous data [6]and was increased to 13.37K by theanneal of 770K, 2000 sec.

    • The RRR values of the ALD NbN filmswere smaller than that of the sputter film.

    5. Conclusion• We succeeded in depositing a 50 nm - thick NbN film on M-plain sapphire with

    relatively high TC of 12.35 K.• The anneal certainly changed the crystal structure conditions of the ALD NbN

    films and the TC was improved up to 13.37 K.• It is considered that the enlargement of the grain size of the NbN by the anneal

    process was occurred by an agglutination of many NbN crystallites, not by thecrystal growth of each NbN crystallite.

    • It is necessary to perform the further investigation in order to decide theoptimal anneal condition of the ALD NbN films.

    This work was supported by JSPS KAKENHI Grant Number 15H03599. A part of this work was conducted at the AIST Nano-Processing Facility.

    AcknowledgmentThe authors thank H. Yamamori and S. Shiki for their help with the experiments, and the clean room members of analog-digital superconductivity (CRAVITY) forperforming experiments.

    6-16am-Poster-2

    Pea

    k inte

    nsi

    ty (

    cps)

    δ-N

    bN(1

    11)

    δ-N

    bN(2

    00)

    δ-N

    bN(2

    20)

    β-N

    b2N(1

    03)

    δ-N

    bN(3

    11)

    δ-N

    bN(2

    22)

    δ-N

    bN(4

    00)

    γ-N

    bN(1

    10)101 011

    110

    1-10 -110

    10-1 01-1

    別2

    別1別1

    別2

    別2別2

    別3

    別3 別3

    別3

    0.00E+00

    5.00E+02

    1.00E+03

    1.50E+03

    2.00E+03

    2.50E+03

    3.00E+03

    13.00 13.20 13.40 13.60 13.80 14.00

    Resi

    stiv

    ity

    (ohm

    )

    Temperature (K)

    Development of NbN films by atomic layer deposition for Superconducting Tunnel Junction particle detectors with a high operating temperature�M. Ukibe, and Go Fujii�National Institute of Advanced Industrial Science and Technology, 1-1-1, Umezono, Tsukuba, Ibaraki, 305-8568, JAPAN