    !
" #$ %&'()+*,.-0/132465
798;:<>=@?ABDC.E.FGH?A.I.JLK@MNOHP@QLR>SLT@I.JULVGHWLXR@YLZD[J.\L]>^_GDI.JLR`aD\@b.c.bdLe>fgh M@I.JLij@kO fg TWl@Y.M@I.JLR>m.cn>o ep@q.r ULVG>YLZ>I@sBLODYt@TWu>R@YLZM<=@?ALv@URI.JLi>wx.y@z e{| ]>} h M[J.\LRI.JLK>~w>@.>>.]>GlWLlMbc.L>RQ.J@o e{| ]@ h TGHW Y e M<=@?ALR.@@R> d K {| ]DLTW.¡]M.<=@?ALK@M¢.£¤UK¥¦§ Lg Y.¨@I©§I. e ¦§LULVM<=Lv.Rª.=.¤@wx.y@zBH«L¬
FGH­U®@¯°t±.²@³DtLGHW´¶µ ·¸ «¬ULK@M¹Dº».a¼@I..½]L.G<=.?ALR0¾À¿ Á Â Ã¹Dº»DR@¨.I©§LI.B>^utWu  ]LMÄ b.c@ÅLÆ@Ç.ÈRAÅLÆULVGHÉLÊLËLa.»@]>T  RÌ@Í e>Î Ï GHWÐ]M@¾À¿ Á Â ÃÑ¹Dº»HRÒ@Ó^HÔÕ
Ó.Ö@×.Ø]>T @Ù.Ú M.X  ]DÛ0ÑÉÊËLa.»RÜ.Ý@³Þ>ßÀà@áRâ@ãBDä@å   TG@æç.èé.êBH©ëFGW
ìîí;ïð;ñ
ò.ó ]Dôõ  Y<>=@?ALR ¾À¿ Á Â ÃÑ¹Hº»HRÒ@Ó.Ö.×@Ø]@n>FG«L¬.UK@M@Ò@Ó.â@ã]DÛ0ÑöL÷.RDÕÓâ@ã
BDø  TGHWu  K>®.ù]>ú û.üu e>ý  h M.XuDUKþ@ÿ.ùL°t>o BDzLT.Y Ú ØL° ë] >Z TGWLõ  õ  KuDR B@ M¾À¿ Á Â Ã ¹Dº»HLRÒ@Ó@Ö.×.ØB I.Jo@ÕÓ Ú  R .U Ù.Ú FGHWu  ]MDÒÓ@Ö.×@ØB @ù.FG L]Õ.ÓâãB .FG  e h MH®@ùL°]Dú  LT  h tLGWlY@MHÕÓR LtLGHöL÷LB "!#.z $ M@¾À¿ Á Â ÃÑ¹Dº»RDÕÓ.Ö.×.Ø]>T  &O % Ù FGHW')( *,+.-0/01325476980:<;=?>A@0BDC.E0F<>=@?A.ÐLG R.°L]HLI °t>ØPBHN fJ K z.FG>YLZ.]LODM@..Ð@ØR {| ]L  YöL÷LB MNFGu eO  ULVGHW..Ð@ØRL  YöL÷DK@M@.PQ BDô0ÀR] .R ILt S ëDmT"UV B G MWLX °.MCY °.t Z[ e \ t@T@]L@G]^`_ a R@¨@Tb öL÷.ULVGHWu Ï R Z[ K@M@R cd M
e R fLg R h`i Dt
G j _Ut h M kLX °tÐ@ØOl h FGHWÐ]M@¥"m@Ø]L@GH d R n e po á°tO>R@ULVGHWPLR.ÐØB  Y<=@?ALRy@EK@M.¨@I©§I.LRq Ut h M {| ]DLT dLe r  G@s öt ]@n>FGuz]L D OÀN O  R v"Lw ° x"L ULVGW<=?ALRDÉ.³`@y RDöL÷@yE]D^T "O L tu.DK Lz R@{ \UVGW| ¥ Ä}~ ÓR | Z[ Lq R`) 000073 w" E ½LR. \LK@M<=@?A@öL÷LBYÇ.ÈLU  w` Ï E & GD\ULVM ×R ½@{.| ]  Y@.°@Ð" B  Y@öL÷LBDy@ELU g GHW) .5D3¡0¢0
@"£ P`.¤ ]>^T  M.¨"s@ÓR ¥»¦A§Àß¨@ß}T¦LaDßLËLR>×©R".U@M{@LRA§ß¨@ß.LR ª.m.o«Le £ PLRL¹Dº».ª m.o]¬  h t  Y g ] ­ >GL¦ aDßLË@s ÓR ®°¯ ±
² ¹Dº»³´µ B¶ z Y@I.½.ULVGHWu>R  ½UK@M ·¸ R m de¹ ¡Yºt {»¼ R>É3½y¾ ¹@¿ ».À R  T »¼Á RLaDß.§ »"Â¼ Ã`y7Ä ³ e>Î ÏÀ Gu>]@tLGHW) Å,¡0¢?Æ97Ç3È0É.Ê7ËÌ0Í ] ¸ «L¬.UzT.YL¹Hº»@a¼>I@"ÎÏLRÐBÑ.FW¥» ¦>.  m Í Ò Í Ó Ô Õ R3ÖØ×@ÅÆ3ÙÚÜÛ3§Àß@¨ ß.M¦ aDßLË> ÝÞ"» b"ß ]L Dà Ú ã  Y>mDá â ã Ô Õ R0ÖØ× BDzT.YW@ä R.å b.m" KM@Xæ  º.ÊDç ³.è »@é m"Lê ]L D MDm" I>©.§5ë ì ë ë ë Í Ô Õ R@í ÓU@±.èî   TLGW@ª m.o"ï.ð KM"¦ aHßËLä ULVG3ÖØ× R ÝÞ» b"
ß BDC.E   TG"¾`§ ßñA.ò »"@¾ R .ó ÓBHô Ü`>õ A.JUö"÷ FGuHUô > TGHWÖØ× R .å b.]>T  K.M.ª m.oï`ðLø ]"Lù »">¾ ³ú ±.ß5À ULVGuBûü FGYLZ>L¼ÃAy7Ä ³`ý"þ
¹DÊL¨ ]L > ±èî   TGHW"ÿ R`§ ß@¨ ß.LRB¡  öL÷L]@U p M     v.R>öL÷
B ò Y9§ ß@¨ ß.B"¦ é.ê@U@I_DML¦ aDßLË@s ÓRâ@ãBDÄ Ê@ß5ÑÀ U>FGHW..â
ö"ßD!Ú #"BDzLT  ¥ »>¦ ] Í ë ë $#%!&R@s Óâö B" _GuU.Ma½>y Ê»'.m   TGHW{ (.wa½ yÊ» Lý »¦ U) d Y*+LR"ýþ a"¾ ,B9#Ú - × .ßDÀ B/0Y213]54 6#çßLË>³B 78 ².ß
>î ú Î è 7Ä ]L  M@²:9Dî ³;<   TGHWu>R.ù ¼Lñ ê.RI©§K@ML¦ aDßLËä ULVG.ÖØ× R .ª m.o
9A½>î ßU=l  ^ M"ã "%!& >  ¹ ? O ÏÀ GHW@í;ïBADCÅ) E .5D02FHGJI#K
.Ò]>^T @Î ÏÀ Y¹Dº»a¼.¼ Ã9y7Ä ³B Ì ã]Ñ.F@WÒ@Ó?â ì L $]>^T MN:M@d â ì Í "%!&DDt >GHW Ù.Ú " K@M`¯ ¥ »>¦ s Ó Ò â Õ O M L¦ aDßË"@s Ó Í Í Õ O M µ a½>y Ê»Lý » .¦ Rø Ú o Í ë ë Õ  M.ª m@oï`ð0â ë ë "%!& - P â  Q RULVGHW 7 K Ù.Ú ².ß`.î BaDß3§ »"Â ò&½ñA@ò »
¾ YO>R@ULVM Î ÏÀ YL¼ ÃAy
Ä ³ e @LaDß.§ »"ÂL
é ULVGu Ï M·¸ R m d B% Ù U g TGu e IL GHWÅ) TS2UWVYX2Z¹Hº».a¼.¼ ÃAy7Ä ³RÒ@Óâ@ã]>T @Ù.Ú Yö[B Ì0Ò ]Ñ.FWÒ@Ó­\] q    dLe ) f FGL@O>]M¹Dº»H e Ë>³ßù 7Ä FGu e õL GHWl@Y.M>©] Yö[LM^ Ù@Ú Ò@Ó_`]>^T  ¼ ÃAy7Ä
Ì a ]M@­UÑ Y¼ÃAy7Ä ³BH©] M¼ ÃAy7Ä ³LRÒ@Ó.Ö.×.ØB¾ ¹
³ e @LaDß.§ »"ÂLé ULV  Y@W W    ! " # $ " #áãâ ä × åÛæ ç æ è ß à '     qd  ¡ ¢£d¤q¥  £§¦  ¨ ©   ª ¤ «  ¦ ¥  ¡ ¨ ¬ ­   ®
¯ ° ± ' ¯ ²  ¢ ® ³ ­ ¬ ° ­ ´  µ§± ­ © ¢ ® d  ¡ ¢Í Î Ï ÐÑ ÒÏ Óøù ú û üîû ý û þ   dd      ¶ ·¸ ¹ ¹º ·¸ »¼

3 4 5 674 5éê ë ì íîì ï ì ðm n oqp r s t u) ) '$(ñ òó ô ôõ òó ö÷ Í Î Ï ÐÑ ÒÏ Óbdc e f g h c e} ~ y     i!c g g h gÿ   §Ô Õ Ö ÿ      m v wqx y z {% | & '$(j gckl  

* + , - .0/ 1 / 2 - .
34 / 674 5½ ¾ ¿ÀÁ Â Ã
Ä ¾ Å Á ¿Æ Ç ÈÉqÊ Â Ã Ë Ì Å Æ× ØqÙ ÚÛ'Ü Ý Þ ß à

Ì98 : ¹Dº».a¼.¼ÃAy7Ä ³ Ù.Ú ÎÏIntensity [a.u.]

HWHM = 5.1 MHz ( 5.7 K )

-40

-200;

2040

Raman Detuning δω/2π [MHz]Ì=< : ¹Dº».a¼.¼ ÃAy7Ä ³?> 7 KLaHß.§»"Â@n>o]L@Gò&½&ñ9ò@»¾DöA@.W4149.64

4149.684149.66
5.7 K

Solid p-H 2 Q 1 (0): Constant Volume
7.0 K

Intensity (arb. units)

1.2

7.9 K

1.4

9.0 K

2.1

10.2 K

3.2

4.9

11.0 K
7.8

4149.644149.66

12.0 K
4149.68

Raman Shift (cm -1 )

Ì=B C ¹Dº»¼ ÃAy0Ä ³RÒ@Óâ@ã]ÀY>öA@BÑ@FWu>R Ì  Ï ÒÓâã]HÛ0DFE G@ßßRIk Ht>w.x.yzR>âãB% Ù U g> TLG.u eõGHWl@Y.Mù7ÄÀ d R  eFJK tâ@ãB  TGu@O ¹    GHW
LNM OQPSRUTWVSX.Õ ÓRLtLG B LR>ö÷RÒ@Ó.Ö.×.ØB"¦La½9ÄHYO>R eÌSY ULVGHW@ÕÓR) f ]DÛT¹Dº»H e ÜÝ@³Þ>ßZ].@\[@ô]"ù7ÄH  TGu. e õLGHW]_^a`ÒÓ.Ö.×.ØB.ù.FG L]@K@MÉÊLËLa@»LIb.» ¯ ^HÔXRFcRAÅLÆ"µDR>wx.y@zBõ.t_ d t Ï t@TW  Ht eÏ M» ÀÑR d KMHN f U
R fhgi R Ä b@cÅÆÇ.ÈUkO j l mFnpoq@ÓUVM.u  K¹Hº» ù0ÄFrkj$i Y s t u npoe É3R s v i wxq@ÓLULVGHW» Ài>.FR yAzA{]L  MÉ3» À)\|WR }hg s R>ÉÊLËLa.» .\n ~HtTW
e l@Y.MÉ3
HT  7  Ï MÉ0» ÀB Á E.FGuL>]L.G¼ ÃAy7Ä³R@Ò@ÓÖ.×.IØ LFR K H  T.ULV  WLXuDU.M
A\IA\AA\\AI\AA HT {| "] ù» ¦>³t±.²@³B A  qYW¹Dº»¼ ÃAyDÄ ³RÒ@ÓÖ.×.ØK@M¹Dº» ù7ÄA¡ ¢ £ K Ib.»\R ¤.c]L@GDb.cÜ.Ý@³Þ>ßLFR ¥  M
d ¦ ¡ ¢ £ K b»@B ¨ HY@I.J@b.cÇ.ÈR Ä (LAw ©ª]>IÆ «  TG>Mh ¬ Ú   X  æ@ êA­.F¹Dº»H §4149.70

55
504149.684149.674149.664149.654149.64

45
40
35
30
25201510504149.63
3 4 5 6 7 8 9 1011121314

3 4 5 6 7 8 9 1011121314
Temperature [K]Temperature [K]Ì§¯$° ¹Dº»ù7Ä±  d RÒ@Ó.Ö.×.Ø

4149.74
density ² [g/cm ] (crystal grown at)-28.665 *10 (24atm)-28.680 *10 (28atm)-28.695 *10 (32atm)
34149.72

Raman Shift [cm -1]

Raman Shift [cm-1]®

Raman Width HWHM [MHz]4149.694149.704149.684149.664149.64³4681012

Temperature [K]Ì=´ ° ¹Dº»ù0ÄÑRDÕÓ.Ö.×.Ø

14

4149.70

5550Raman Shift [cm-1]®

Raman Width HWHM [MHz]4149.694149.684149.674149.664149.654149.64454035302520151054149.63
3 4 5 6 7 8 9 1011121314
Temperature [K]0

3 4 5 6 7 8 9 1011121314
Temperature [K]Ì=µ ¶378 öA@®.ùDR·°¯ ¸)¥¹@æ>ß`îò½&ñAò.»"¾ µGLMu Ï K>öA@L°L] Lz RÀtU¹L_Gu e õL GHWº» ¼ ½¿¾ÁÀÂAÃ ¼¼$ÄÅ ÆpÇAË È ÉÊ È Î ÏhÌ ÐIÍ Ñ$Ò ÌÎÏÓ » ¼ ½¿¾ÁÀxÔ Ã ¼¼$ÄÅ ÕpÇ Ë È ÉÊ È » Î ÏhÌ$Ö ÐIÑ ½ × Ò
Ì
78 @ ò&½&ñ`ò "¾ ÌUµò&½&ñAò "¾Ø ç 2 ¾IÙyî U¸NÚ ¥`îù7Ä±"o78 A@\ÛkÜÑù7Ä µÀÂAÝßÞ ¯AàêAá
"³,°¯µãâ Fä å µæ»Ñ½»¸ ½u Ï RDo BHzLT  M ö ]@» .B _>YO>R e ULVGWu>R» U.K@M Ú oH¼ >ß D»>ßR R ¹æ>ß @]L D d @O>] {| ]@T e>Î Ï ^M±.²@³R DØB   TGOR ¡ ÏÀ GHWl@Y.M ö D hË>³LßULVGLu
@OÀo L°L]  YW Ï ]M>ÕÓ.Ö@×.Ø]@n  ODM@I.JLi.R>wx.y@z e I.J@b.ci.RIj@kR]]L@GO>R@ULVGL Ú FGuHU Ú Q°L] ë@U g GHW
ç_èaé@I J@oÕÓ Ú R.U@MFêhë » Þ ½ ¹Dº»HLRÒÓ=± ÕÓ.Ö@×.ØLR Ù@Ú BDô  Y>Wêhë » Þ ½ ¹Dº»HLRÒÓ.Ö@×ØBë>FGD±.²@³  I.J@b.c²ÉÊIb.»LDR>wx.y@z  BH©ì ÀM 78 ².ß`î· YWLXR>ö @LM ¹Dº» ª.m.oK@:M b»D¤LR íÜ.Ý@³Þ>ß] å   Ò@ÓA­ î]DÛT ) f FGuHM ¹Dº»Hd K:M Ib.»@]L@GHÉÊLËLa.»R Ä (w ïð]L  Ò@ÓA­ î]DÛLT ) f FG.u>B@ë Ï ]YWÒ@ÓÕÓ]L@G ñA@B>I@kLU g YuHU.M {| ]@\ë òLt>ö.ù e>Î ÏÀ YHTL¡GHW>@­LR]@¼ ÃAy7Ä ³"B ùL» ¦>³] Lë@U g GR.K@M<=@?A]>^T  ÉÊËLa.»L Ib.» e @F óIô]DbG õ  TGu>B $Iö  TGHWu  K@MC.EI.J \e ÷ ô@I.JLRQ.J@ØB    TG<=@?A]>^T KMO  @O Ï T@"Ð L°t>Aö @HTL¡.G jIøWùLF
R ú\  Ï K@M¹Dº».a¼.¼ ÃAy7Ä ³ e y@E YöL÷R>o ®t@\T ûAü½LR @ @{| F] ý@zLULVGu>B ûüYW
þAÿ  d Ib.
» > Ý RÆ]L@G Ä (Aw ïð RLRD©ë » ]M¨ í.ÓtDÕÓ.Ö.×.ØR Ù.Ú 
Ú Q.°tD© ì e R x"ULVG