38 Te(OH) 6 2NH 4 H 2 PO 4 (NH 4 ) 2 HPO 4

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1 Fig. A-1-1. Te(OH) NH H PO (NH ) HPO (TAAP). Projection of the crystal structure along the b direction [Ave] ( a a )/ a [1 ] ( b b )/ b [1 ] ( c c )/ c [1 ] Angle β Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). (a a )/a, (c c )/c, (b b )/b, β vs. T [9Prz]. a, b, c : extrapolated values of a, b, c, respectively, from the phase I.

2 5 κ 1 Dielectric constant κ 1 [1 ] 1 κ κ Dielectric constant κ, κ [1 ] Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). κ 1, κ, κ vs. T [91Cza]. κ 1 : dielectric constant for E parallel to the polar direction, κ 1 κ (11). κ = κ b. κ : dielectric constant for E along the direction perpendicular to both the polar axis and the b axis. Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). κ a, κ b, κ c, κ 1 1 a, κ c vs. T [Gui].

3 . Inv. dielectric constant κ (11) [1 ] 1 1 f = 1 khz Conductivity σ [1 Ω m ] Fig. A-1-5. Te(OH) NH H PO (NH ) HPO (TAAP). κ, σ vs. T [9Cac]. κ (11) : dielectric constant perpendicular to (11). σ: ac conductivity. f = 1 khz.. 1 (11). 1 Dielectric constant κ (11) [1 ] Temperature T [ C] Fig. A-1-. [Te(OH) NH H PO (NH ) HPO ] 1 x [Te(OD) ND D PO (ND ) DPO ] x. κ (11) vs. T [Sha]. 1: x =, : partially deuterated, : x 1. κ (11) : dielectric constant for E perpendicular to (11) face.

4 15 1 (11) [1 ] Inv. dielectric constant κ Temperature T [ C] Fig. A-1-7. [Te(OH) NH H PO (NH ) HPO ] 1 x [Te(OD) ND D PO (ND ) DPO ] x. [Sha]. 1: x =, : partially deuterated, : x 1. κ 1 (11) vs. T f = 1 khz 1 (11) [1 ] Inv. dielectric constant κ 7 5 p = 5. 1 Pa Pa Temperature T [ C] Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). κ vs. T [9Fer]. Parameter: p. 1 (11)

5 Dielectric constant κ (11) [1 ] T = C (11) [1 ] Inv. dielectric constant κ Pressure p [1 Pa] 1 Fig. A-1-9. Te(OH) NH H PO (NH ) HPO (TAAP). κ (11), κ vs. p [9Sha]. T = C. f = 1 khz. (11) T = 9 K f = 1 khz 1 (11) [1 ] Inv. dielectric constant κ Pressure p [1 Pa] Fig. A-1-1. Te(OH) NH H PO (NH ) HPO (TAAP). κ vs. p [9Fer]. T = 9 K. 1 (11)

6 Transition temperature Q f [ C] 1 5 Pressure p [1 Pa] Fig. A Te(OH) NH H PO (NH ) HPO (TAAP). Θ f vs. p [9Sha]... R = min min 9 min 15 min Dielectric constant κ (11) [1 ] Temperature T [ C] Fig. A-1-1. Te(OH) NH H PO (NH ) HPO (TAAP). κ (11) vs. T [91Sha]. Parameter: R. R: irradiation time of X-ray. X-ray from Cu target of kv, 5 ma was used.

7 f =5MHz 9 MHz Dielectric constant κ'[11] [1 ] GHz MHz GHz.5. GHz 15 GHz 77 GHz Fig. A-1-1. Te(OH) NH H PO (NH ) HPO (TAAP). κ [11 ] vs. T [9Sob]. Parameter: f. κ [11 ] dielectric constant for E [11]. : real part of

8 7 f = GHz MHz Dielectric constant κ''[11] 5 9 MHz GHz GHz. GHz 15 GHz 1 5 MHz 77 GHz Fig. A-1-1. Te(OH) NH H PO (NH ) HPO (TAAP). κ [11 ] vs. T [9Sob]. Parameter: f. κ [11 ] : imaginary part of dielectric constant for E [11].

9 1. T f =. K Dielectric constant κ'[11] [1 ] 1... K 1.5 K Frequency f [Hz] Fig. A Te(OH) NH H PO (NH ) HPO (TAAP). κ [11] vs. f [9Sob]. Parameter: T Θ f. T f =. K Dielectric constant κ''[11] K 1.5 K Frequency f [Hz] Fig. A-1-1. Te(OH) NH H PO (NH ) HPO (TAAP). κ [11] vs. f [9Sob]. Parameter: T Θ f.

10 1 Dielectric constant κ''[11] f =. GHz GHz 1. K. K GHz 1. K. K 5GHz Dielectric constant κ' [11] T f =.5 K MHz 1 MHz 5 MHz Fig. A Te(OH) NH H PO (NH ) HPO (TAAP). κ [11] vs. κ [11] (Cole-Cole diagram) [9Sob]. Parameter: T Θ f, f. Cross: center of circular arc. 15 [1 s ] ( πτ ) Fig. A-1-1. Te(OH) NH H PO (NH ) HPO (TAAP). (πτ) 1 vs. T [9Sob]. τ: dielectric relaxation time.

11 Dielectric constant κ (11) [1 ] 5 1 f = 1 khz 5.5 E bias = 9. 1 E bias = 1. 1 V m V m Fig. A Te(OH) NH H PO (NH ) HPO (TAAP). κ (11) vs. T [9Cac]. Parameter: E bias. κ (11) : dielectric constant for E perpendicular to (11) face. Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). P s, P s vs. T [Gui]. P s : spontaneous polarization measured on (11) plate.

12 . 1.5 Polarization P s [1 C m ] Fig. A-1-1. Te(OH) NH H PO (NH ) HPO (TAAP). P s vs. T [9Cac] ( P / P ) [1 ] s s.. 5 Temperature T [ C] Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). (P s / P s ) vs. T [9Fer]. P s : saturated spontaneous polarization: P s =.1 1 C m.

13 .. Polarization P s [1 C m ] Pa p =1. 1 Pa Temperature T [ C] Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). P s vs. T [9Sha]. Parameter: p.. p =. Polarization P s [1 C m ] p = 1. 1 Pa Pa 1 1 Reduced temperature T [K] Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). P s vs. T Θ f [9Sha]. Parameter: p. f

14 1. T =.5 K 1. ( P / P ) [1 ] s s Pressure p [1 Pa] Fig. A-1-5. Te(OH) NH H PO (NH ) HPO (TAAP). (P s /P s ) vs. p at.5 K [9Fer]. P s : saturated spontaneous polarization; P s =.1 1 C m. 5 1 Pyroelectric coefficient p 1 [1 C m K ] Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). p 1 vs. T [91Cza]. p 1 : pyroelectric coefficient measured perpendicular to (11) face.

15 1 1 Specific heat c p [1 J K kg ] Fig. A-1-7. Te(OH) NH H PO (NH ) HPO (TAAP). c p vs. T [Gui]. c p : specific heat capacity at constant pressure. Circle: adiabatic calorimeter method; plus sign: pyroelectric method. ( υ υ o )/ υ o [1 ] 1 f =1MHz MHz 5 MHz Temperature T [ C] Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). (υ υ )/υ vs. T [91Ban]. Parameter: f. υ: longitudinal ultrasonic wave velocity perpendicular to (11). υ : υ at 1 C.

16 5 f =1MHz MHz 5 MHz 5 15 Attenuation α [1 db m ] Temperature T [ C] Fig. A-1-9. Te(OH) NH H PO (NH ) HPO (TAAP). α vs. T [91Ban]. Parameter: f. α: attenuation coefficient of longitudinal ultrasonic wave perpendicular to (11) face. c n P s 5 b n β 1 =5 n 1 a Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). Orientation of principal axes of optical indicatrix [9Prz, Gui]. Rotation of the optical indicatrix with temperature: see Fig. A-1-1.

17 .7..5 Rotation angle θ [ ] Temperature T [ C] Fig. A-1-1. Te(OH) NH H PO (NH ) HPO (TAAP). θ vs. T [Gui]. θ: rotation angle of optical indicatrix. See Fig. A ( n 1 ) [1 ].... δ ( n 1 ) [1 ] Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). ( n 1 ), δ( n 1 ) vs. T [9Prz]. λ =. nm. ( n 1 ) = n 1 (T) n 1 (9 K), n 1 = n n. δ( n 1 ): deflection of n 1 from that of the extrapolated values of phase I. n 1, n, n : principal refractive indices. See Fig. A-1-. Full line: extrapolated value from the phase I.

18 1 1 δ ( n ) [1 ] 5 δ ( n ) [1 ] Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). δ( n ), δ( n ) vs. T [9Prz]. λ =. nm. δ( n i ): deflection of n i from that of the extrapolated values of the phase I. n = n n 1, n = n 1 n. n 1, n, n : principal refractive indices; see Fig. A-1-. Fig. A-1-. Te(OH) NH H PO (NH ) HPO (TAAP). ν vs. T [Gai]. ν : 1 P chemical shift. ν L = 1 MHz.

19 1 1 Inv. time t m [1 s ] T = 7.7 C C Electric field E [1 Vm ] Fig. A-1-5. Te(OH) NH H PO (NH ) HPO (TAAP). t vs. E [91Sha]. Parameter: T. t m : time corresponding to the maximum switching current. 1 m

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