We have experimentally performed the coherent control of delocalized ro-vibrational wave packets (RVWs) of solid para-hydrogen (p-H2) by the wave packet interferometry (WPI) combined with coherent anti-Stokes Raman scattering (CARS). RVWs of solid p-H2 are delocalized in the crystal, and the wave function with wave vector k ∼ 0 is selectively excited via the stimulated Raman process. We have excited the RVW twice by a pair of femtosecond laser pulses with delay controlled by a stabilized Michelson interferometer. Using a broad-band laser pulse, multiple ro-vibrational states can be excited simultaneously. We have observed the time-dependent Ramsey fringe spectra as a function of the inter-pulse delay by a spectrally resolved CARS technique using a narrow-band probe pulse, resolving the different intermediate states. Due to the different fringe oscillation periods among those intermediate states, we can manipulate their amplitude ratio by tuning the inter-pulse delay on the sub-femtosecond time scale. The state-selective manipulation and detection of the CARS signal combined with the WPI is a general and efficient protocol for the control of the interference of multiple quantum states in various quantum systems.

1.
I.
Neder
 et al,
Nature
448
,
333
-
337
(
2007
).
2.
O.
Carnal
and
J.
Mlynek
,
Phys. Rev. Lett.
66
,
2689
(
1991
).
3.
D. W.
Keith
,
C. R.
Ekstrom
,
Q. A.
Turchette
, and
D. E.
Pritchard
,
Phys. Rev. Lett.
66
,
2693
(
1991
).
4.
L.
Hackermüller
 et al,
Phys. Rev. Lett.
91
,
090408
(
2003
).
5.
T. C.
Weinacht
,
J.
Ahn
, and
P. H.
Bucksbaum
,
Phys. Rev. Lett.
80
,
5508
(
1998
);
T. C.
Weinacht
,
J.
Ahn
, and
P. H.
Bucksbaum
,
Nature
397
,
233
(
1999
).
6.
R. R.
Jones
 et al,
Phys. Rev. Lett.
71
,
2575
(
1993
);
[PubMed]
R. R.
Jones
,
Phys. Rev. Lett.
75
,
1491
(
1995
).
[PubMed]
7.
L. D.
Noordam
,
D. I.
Duncan
, and
T. F.
Gallagher
,
Phys. Rev. A
45
,
4734
(
1992
).
8.
R. E.
Carley
 et al,
J. Phys. B: At., Mol. Opt. Phys.
38
,
1907
(
2005
).
9.
D.
Meshulach
and
Y.
Silberberg
,
Nature
396
,
239
(
1998
).
10.
T.
Brixner
,
G.
Krampert
,
T.
Pfeifer
,
R.
Selle
,
G.
Gerber
,
M.
Wollenhaupt
,
O.
Graefe
,
C.
Horn
,
D.
Liese
, and
T.
Baumert
,
Phys. Rev. Lett.
92
,
208301
(
2004
).
11.
B. J.
Sussman
,
D.
Townsend
,
M. Yu.
Ivanov
, and
A.
Stolow
,
Science
314
,
278
(
2006
).
12.
K.
Ohmori
,
H.
Katsuki
,
H.
Chiba
,
M.
Honda
,
Y.
Hagihara
,
K.
Fujiwara
,
Y.
Sato
, and
K.
Ueda
,
Phys. Rev. Lett.
96
,
093002
(
2006
).
13.
H.
Katsuki
,
K.
Hosaka
,
H.
Chiba
, and
K.
Ohmori
,
Phys. Rev. A
76
,
013403
(
2007
).
14.
H.
Katsuki
,
H.
Chiba
,
B.
Girard
,
C.
Meier
, and
K.
Ohmori
,
Phys. Rev. Lett.
102
,
103602
(
2009
).
15.
N. F.
Scherer
 et al,
J. Chem. Phys.
95
,
1487
(
1991
).
16.
V.
Blanchet
,
M. A.
Bouchene
, and
B.
Girard
,
J. Chem. Phys.
108
,
4862
(
1998
).
17.
A.
Monmayrant
,
B.
Chatel
, and
B.
Girard
,
Phys. Rev. Lett.
96
,
103002
(
2006
);
[PubMed]
A.
Monmayrant
,
B.
Chatel
, and
B.
Girard
,
Opt. Commun.
264
,
256
(
2006
).
18.
R. A.
Bartels
,
T. C.
Weinacht
,
S. R.
Leone
,
H. C.
Kapteyn
, and
M. M.
Murnane
,
Phys. Rev. Lett.
88
,
033001
(
2002
).
19.
M.
Leibscher
,
I. S.
Averbukh
, and
H.
Rabitz
,
Phys. Rev. Lett.
90
,
213001
(
2003
).
20.
H.
Stapelfeldt
and
T.
Seideman
,
Rev. Mod. Phys.
75
,
543
(
2003
).
21.
F.
Rosca-Pruna
and
M. J. J.
Vrakking
,
J. Chem. Phys.
116
,
6567
(
2002
).
22.
M.
Spanner
,
E. A.
Shapiro
, and
M.
Ivanov
,
Phys. Rev. Lett.
92
,
093001
(
2004
).
23.
C.
Horn
,
M.
Wollenhaupt
,
M.
Krug
,
T.
Baumert
,
R.
de Nalda
, and
L.
Bañares
,
Phys. Rev. A
73
,
031401(R)
(
2006
).
24.
E. W.
Lerch
,
X.
Dai
,
S.
Gilb
,
E. A.
Torres
, and
S. R.
Leone
,
J. Chem. Phys.
124
,
044306
(
2006
).
25.
K.
Kitano
,
H.
Hasegawa
, and
Y.
Ohshima
,
Phys. Rev. Lett.
103
,
223002
(
2009
).
26.
S.
Zhdanovich
,
A. A.
Milner
,
C.
Bloomquist
,
J.
Floß
,
I. S.
Averbukh
,
J. W.
Hepburn
, and
V.
Milner
,
Phys. Rev. Lett.
107
,
243004
(
2011
).
27.
A.
Korobenko
,
A. A.
Milner
, and
V.
Milner
,
Phys. Rev. Lett.
112
,
113004
(
2014
).
28.
J.
Lindgren
,
E.
Hulkko
,
M.
Pettersson
, and
T.
Kiljunen
,
J. Chem. Phys.
135
,
224514
(
2011
).
29.
M.
Fushitani
 et al,
Phys. Chem. Chem. Phys.
7
,
3143
(
2005
).
30.
A. P.
Heberle
,
J. J.
Baumberg
, and
K.
Köller
,
Phys. Rev. Lett.
75
,
2598
(
1995
).
31.
N. H.
Bonadeo
,
J.
Erland
,
D.
Gammon
,
D.
Park
,
D. S.
Katzer
, and
D. G.
Steel
,
Science
282
,
1473
(
1998
).
32.
D.
Press
,
T. D.
Ladd
,
B.
Zhang
, and
Y.
Yamamoto
,
Nature
456
,
218
(
2008
).
33.
R.
Hildner
,
D.
Brinks
, and
N. F.
van Hulst
,
Nat. Phys.
7
,
172
(
2011
).
34.
F.
Dubin
,
R.
Melet
,
T.
Barisien
,
R.
Grousson
,
L.
Legrand
,
M.
Schott
, and
V.
Voliotis
,
Nat. Phys.
2
,
32
(
2005
).
35.
L.
Legrand
,
A.
Al Choueiry
,
J.
Holcman
,
A.
Enderlin
,
R.
Melet
,
T.
Barisien
,
V.
Voliotis
,
R.
Grousson
, and
M.
Schott
,
Phys. Status Solidi
245
,
2702
(
2008
).
36.
M.
Kuwata-Gonokami
,
R.
Shimano
, and
A.
Mysyrowicz
,
J. Phys. Soc. Jpn.
71
,
1257
(
2002
).
37.
J.
Van Kranendonk
,
Solid Hydrogen
(
Plenum
,
New York
,
1983
).
38.
I. F.
Silvera
,
Rev. Mod. Phys.
52
,
393
(
1980
).
39.
J. Z.
Li
,
M.
Katsuragawa
,
M.
Suzuki
, and
K.
Hakuta
,
Phys. Rev. A
58
,
R58
(
1998
).
40.
I. I.
Abram
,
R. M.
Hochstrasser
,
J. E.
Kohl
,
M. G.
Semack
, and
D.
White
,
Chem. Phys. Lett.
71
,
405
(
1980
).
41.
H.
Katsuki
,
Y.
Kayanuma
, and
K.
Ohmori
,
Phys. Rev. B
88
,
014507
(
2013
).
42.
J.
Cheng
,
A.
Volkmer
,
L. D.
Book
, and
X. S.
Xie
,
J. Phys. Chem. B
106
,
8493
(
2002
).
43.
E.
Goovaerts
,
X. Y.
Chen
,
A.
Bouwen
, and
D.
Schoemaker
,
Phys. Rev. Lett.
57
,
479
(
1986
).
44.
H.
Katsuki
,
K.
Ohmori
,
T.
Horie
,
H.
Yanagi
, and
K.
Ohmori
,
Phys. Rev. B
92
,
094511
(
2015
).
45.
K.
Hosaka
,
H.
Shimada
,
H.
Chiba
,
H.
Katsuki
,
Y.
Teranishi
,
Y.
Ohtsuki
, and
K.
Ohmori
,
Phys. Rev. Lett.
104
,
180501
(
2010
).
46.
Y.
Teranishi
,
Y.
Ohtsuki
,
K.
Hosaka
,
H.
Chiba
,
H.
Katsuki
, and
K.
Ohmori
,
J. Chem. Phys.
124
,
114110
(
2006
).
47.
48.
H.
Katsuki
,
T.
Nakamura
, and
T.
Momose
,
J. Chem. Phys.
116
,
8881
(
2002
).
49.
K. E.
Kerr
,
T.
Momose
,
D. P.
Weliky
,
C. M.
Gabrys
, and
T.
Oka
,
Phys. Rev. Lett.
72
,
3957
(
1994
).
50.
R. A.
Steinhoff
,
K. V. S. R.
Apparao
,
D. W.
Ferguson
,
K. N.
Rao
,
B. P.
Winnewisser
, and
M.
Winnewisser
,
Can. J. Phys.
72
,
1122
(
1994
).
51.
S. K.
Bose
and
J. D.
Poll
,
Can. J. Phys.
68
,
159
(
1990
).
52.
T.
Momose
,
D. P.
Weliky
, and
T.
Oka
,
J. Mol. Spectrosc.
15
,
760
(
1992
).
53.
S. S.
Bhatnagar
,
E. J.
Allin
, and
H. L.
Welsh
,
Can. J. Phys.
40
,
9
(
1962
).
54.
F.
Barocchi
,
A.
Guasti
,
M.
Zoppi
,
J. D.
Poll
, and
R. H.
Tipping
,
Phys. Rev. B
37
,
8377
(
1988
).
55.
56.
S.
Tam
and
M. E.
Fajardo
,
Rev. Sci. Instrum.
70
,
1926
(
1999
).
57.
V. F.
Sears
and
J.
Van Kranendonk
,
Can. J. Phys.
42
,
980
(
1964
).
58.
H.
Goto
,
H.
Katsuki
,
H.
Ibrahim
,
H.
Chiba
, and
K.
Ohmori
,
Nat. Phys.
7
,
383
(
2011
).
59.
C.
Sierens
,
A.
Bouwen
,
E.
Goovaerts
,
M.
De Mazière
, and
D.
Schoemaker
,
Phys. Rev. A
37
,
4769
(
1988
).
60.
D. G.
England
,
P. J.
Bustard
,
J.
Nunn
,
R.
Lausten
, and
B. J.
Sussman
,
Phys. Rev. Lett.
111
,
243601
(
2013
).
61.
K. C.
Lee
,
M. R.
Sprague
,
B. J.
Sussman
,
J.
Nunn
,
N. K.
Langford
,
X.-M.
Jin
,
T.
Champion
,
P.
Michelberger
,
K. F.
Reim
,
D.
England
,
D.
Jaksch
, and
I. A.
Walmsley
,
Science
334
,
1253
(
2011
).
62.
J.
Lim
,
H.
Lee
,
S.
Lee
,
C.-Y.
Park
, and
J.
Ahn
,
Sci. Rep.
4
,
5867
(
2014
).
You do not currently have access to this content.