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1

Department of Physics, University of Basel, Klingelbergstrasse 82, 4056 Basel, Switzerland 2 Institute of Theoretical Physics, Chinese Academy of Sciences, Beijing, 100080, China (Dated: February 1, 2008)

The Stern-Gerlach eect is well-known as spin-dependent splitting of a beam of atoms with magnetic moments by a magnetic-eld gradient. Here, we show that an induced gauge potential may lead to a similar eect for chiral molecules. In the presence of three inhomogeneous light elds, the center-of-mass of a three-level chiral molecule is subject to an optically induced gauge potential, and the internal dynamics of the molecules can be described as an adiabatic evolution in the reduced pseudo-spin subspace of the two lowest energy levels. We demonstrate numerically that such an induced gauge potential can lead to observable pseudo-spin dependent and chiralitydependent generalized Stern-Gerlach eects for mixed left- and right-handed chiral molecules under realistic conditions.

PACS numbers: 03.65.-w,03.65.Vf,11.15.-q,42.50.-p

Introduction. The Stern-Gerlach experiment [1] is one of the milestones in the development of quantum theory. The observation of the splitting of a beam of silver atoms in their ground states in a non-uniform magnetic eld led to the concept of the electronic spin. In this paper we will show that even in the absence of a magnetic-eld gradient, the center-of-mass of certain atoms or molecules in optical elds will follow dierent trajectories corresponding to dierent inner states. This phenomenon is straightforwardly explained as a generalized Stern-Gerlach eect by the optically-induced gauge potential [2, 3, 4]. This induced gauge potential consists of the eective vector and scalar potentials, which result from the adiabatic variable separation of the slow spatial and fast inner dynamics of the atom according to the generalized Born-Oppenheimer approximation [4]. Recently, there has been considerable interest to implement various pseudo-spin dependent induced gauge potentials for cold atoms. Examples include the induced monopole [5], and the spin Hall eect for cold atoms [6, 7], in direct analogy to the spin Hall eect due to the spin-orbit coupling in condensed matter physics [8]. Here, we would like to consider consequences of the induced gauge potential in systems of cold chiral molecules [9, 10, 11] that manifest themselves as a generalized Stern-Gerlach eect. We consider a chiral molecule (see Fig. 1), which is described by a cyclic three-level system [9, 10, 12, 13, 14] where any two of the three levels are coupled by a classical optical eld. A specic example are cyclic three-level (-type) chiral molecules, e.g., the D2 S2 enantiomers in Ref. [10] when only the lowest three states in each well are considered. Such symmetry-breaking systems can also be implemented using an asymmetric well and its mirror [9] (i.e., one asymmetric well and its mirror form a symmetric double well which supports chirality), or a superconducting circuit acting as an eective atom [12]. It will be shown that the optically-induced gauge

potentials for the chiral molecules will be both chiralitydependent and pseudo-spin-dependent when the internal dynamics of chiral molecules are described as an adiabatic evolution in the reduced pseudo-spin subspace of the two lowest energy levels. Thus, the generalized SternGerlach eect can be used to distinguish molecules with dierent chiralities, suggesting a discrimination method to separate chiral mixtures.

Left-handed: Right-handed:

D

W 23 W23

3

W13

W13

W12

-W12

1

(b)

(a)

FIG. 1: (Color online) Model of three-level -type left-(a) and right-(b) handed chiral molecules, coupled to laser beams with Rabi frequencies 12 , 13 , and 23 .

Model. We rst consider a general case of symmetrybreaking molecule having a -type or cyclic three-level conguration (e.g., see the left-handed chiral molecule in Fig. 1(a)). The ground state |1 and the metastable state |2 are coupled to the excited state |3 through spatially varying classical laser elds, with the Rabi frequencies 13 and 23 , respectively. In contrast to the -type system, an additional coupling between |1 and |2 is applied by the third classical laser eld with the Rabi frequency 12 . 3 The total wave function |(r) = j=1 j (r)|j of the cyclic molecule, where r denotes the molecular centerof-mass, is governed by the total Hamiltonian H = p2 /(2m) + U (r) + Hinn , where m is the molecular mass. The trapping potential U (r) = j Uj (r)|j j| is diagonal in the basis of inner states |j , and the inner Hamilto-

2 nian Hinn contains the free terms j |j j| and the Rabi coupling terms jl exp(ijl t) |j l|+H.c. (j = 1, 2, 3; l > j) where j corresponds to the inner level energies. From now on we assume = 1. Here, the frequencies of the three classical optical elds are jl matching the transition |j |l with the Rabi frequencies jl = jl Ejl = |jl (t)| exp(ijl ), respectively; jl are the electrical dipole matrix elements, and Ejl the envelopes of electric elds corresponding to the optical elds that couple levels j and l; jl are the corresponding phases. We now consider the case that the optical eld of Rabi frequency 12 is resonant to the transition |1 |2 , while the other two optical elds are in two-photon resonance with the same single-photon detuning = 3 2 23 = 3 1 13 (see Fig. 1(a)). For position-independent or adiabatically varying jl , the inner Hamiltonian Hinn can be re-written in a timeindependent form

3 Hinn = |3 3| + l>j=1

jl |j l| + H.c.

(1)

with the eective Hamiltonian H = (i+A(r))2 /(2m)+ V (r). Here, the induced gauge potentials, i.e., the vector potential A(r) and the scalar potential V (r), are two 3 3 matrices dened by Aj,l = i j |l and Vj,l = j j,l + j |U (r)|l . The o-diagonal elements of A and V can be neglected: the Born-Oppenheimer approximation can be applied to show that they vanish if the adiabatic condition applies [4]. Furthermore, the inner excited state |3 = |3 , whose eigen-energy 3 = is much larger than the other inner eigen-energies 1 and 2 , is decoupled from the other inner dressed states. Thus, the three-level cyclic system is reduced to the subsystem spanned by the two lower eigenstates {|1 , |2 }, which are robust to atomic spontaneous emission. This results in an eective spin-1/2 system with pseudo-spin up and down states | |1 and | |2 . The Schrdinger equation of the eective two-level syso tem in the pseudo-spin-1/2 basis {| , | } is governed by the diagonal eective Hamiltonian He = H | | + H | |, where 1 (i + A )2 + V (r), ( =, ) . (4) 2m Here, A = i | is the spin-dependent induced vector potential and H = V (r) = + |U | 1 [ | + | | |2 ] (5) + 2m is the reduced optically-induced scalar potential [16] for the spin- component where , := 1,2 . We now consider a specic conguration of three Gaussian laser beams co-propagating in the direction. The z spatial proles of the corresponding Rabi frequencies jl are assumed to be of Gaussian form jl = 0 e(xxjl ) jl

2 2 /jl ikjl z

in the interaction picture. From now on, we assume large detuning and weak coupling: || |13 | |23 | |12 |, so that we can use a canonical transformation [14, 15] to eliminate the excited level |3 from the Hamiltonian (1). To this end we decom pose the Hamiltonian as Hinn = H0 + H1 + H2 with the zeroth-order Hamiltonian H0 = |3 3|, the rst-order term H1 = 13 |1 3| + 23 |2 3| +H.c., and secondorder term H2 = 12 |1 2| +H.c.. Then the unitary inn transformation [14, 15] He = exp(S)Hinn exp(S) H0 + [H1 , S]/2 + H2 dened by the anti-Hermitian operator S = (13 |1 3| + 23 |2 3| H.c.)/ results in the following second-order Hamiltonian

inn He = |3 3| + 1 |1 1| + 2 |2 2|

(6)

+ (gei |1 2| + H.c.),

(2)

where the energy shifts i are given by 1 = |13 |2 /, 2 = |23 |2 /, and the eective coupling is g exp(i) = 12 13 /. The instantaneous eigen23 inn states of He are obtained as |3 = |3 , and the dressed states |1 = cos |1 + ei sin |2 , |2 = sin |1 + ei cos |2 (3)

where j < l = 1, 2, 3, 0 are real constants, the wave jl vectors satisfy k12 +k23 k13 = 0, and the center positions are assumed to be x13 = x23 = x, x12 = 0. The explicit form of the vector potentials are A = k12 sin2 z , A = k12 cos2 z . e e (7)

with the corresponding eigenvalues j = j (1)j g tan for j = 1, 2 and 3 = where is given by tan 2 = 2g/(1 2 ). Induced gauge potentials. In the new inner dressedstate basis {|1 , |2 , |3 }, the full quantum state 3 |(r) = should be represented as j=1 j (r)|j 3 |(r) = j=1 j (r)|j , where the wave functions = 1 , 2 , 3 )T obey the Schrdinger equation it = H ( o

Thus, the dierent spin states of the molecule will have opposite spin-dependent eective magnetic elds B = B according to B = A [17]. The internal state of the molecule is prepared in the spin up and down by using the laser beams. The external atomic trap U (r) is turned o at time t = 0, and the molecules fall due to gravity with an acceleration G along the direction z [18]. The scalar potentials V for spin-up and down molecules are given explicitly as 1 2 [k sin2 (1 + sin2 ) + (x )2 ], 2m 12 1 2 2 V (r) = + [k cos2 (1 + cos2 ) + (x ) ]. 2m 12 V (r) = +

(8)

3 The spin-dependent induced vector potential A (r) and scalar potential V (r) lead to the following equations of orbital motion x = p,x p,x p,z A,z , z = , p,z = mG, m m 1 [(x A,z )p,z A,z x A,z ] x V . = m

(9)

Hence, there will be a Stern-Gerlach-like eect, i.e., different spatial motion of the cyclic molecules corresponding to dierent initial states of spin up and down. In contrast to the standard Stern-Gerlach eect, the eective magnetic eld is not required to have a gradient. Here and in the following, we treat the orbital motion as classical because of the large molecular mass and weak eective gauge potentials. Generalized Stern-Gerlach eect. In the large detuning and weak-coupling limit, the above approach works well for any type of cyclic three-level system. It can also be applied in an experimentally feasible scheme to detect the chirality of molecules, since the left- and right-handed molecules have dierent Stern-Gerlach-like eects. Physically, left- and right-handed molecules have the same intrinsic properties except the antisymmetry of the total phase for the three coupled Rabi frequencies [9, 10]. Hence, we can dene L ij as the Rabi frequenij cies for the left-handed molecules, and dene the Rabi frequencies for the right-handed ones: R 12 and 12 R 13 , R 23 for the same coupling optical elds 13 23 (see Fig. 1(a,b)). Therefore the dierence in chirality leads to two dierent eective couplings, gL/R eiL/R = 12 1 13 , 23 (10)

FIG. 2: (Color online) Schematic illustration of the generalized Stern-Gerlach experiment of oriented chiral molecules. (a) Mixed chiral molecules trapped by the external potential U (r), are coupled to three laser elds and reduce to the lower dressed internal state-space of spin-up and spin-down. (b) After the trap potential is switched o at time t = 0, the molecules will fall under gravity G = 9.8 m/s2 . Due to the chirality-dependent induced gauge eld, molecules with different chirality will experience dierent Stern-Gerlach eects.

(the rst indexes of the l.h.s correspond to the above symbols of the r.h.s.) which results in two dierent eective inner Hamiltonians He

inn(Q)

= |3 + (gQ e

QQ iQ

3| + 1 |1 |1

QQ

1| + 2 |2

2|

Initially, the mixed left- and right-handed oriented molecules, which are spatially conned due to the external trap potential, are subject to the three coupling optical elds as seen in Fig. 2(a) and reduced to the spin-state space {| L/R , | L/R }. At time t = 0, the external trap potential is turned o and the molecules will fall due to gravity. As in the above consideration for the general case of cyclic-type molecules in Eqs. (2)(9), we can obtain the optically-induced potentials and molecular classical trajectories for left- and right-handed molecules, respectively. This is schematically illustrated in Fig. 2(b), which shows that the generalized SternGerlach eect splits the initial cloud into four subsets, since the eective gauge potentials depend both on spin and chirality.

To make this picture of a generalized Stern-Gerlach eect more quantitative, we show in Fig. 3 the typical position of an oriented ensemble of mixed left- and righthanded molecules and spin states subject to gravity (in the z -direction). For temperatures below 1 K, the initial velocity of the molecules can be neglected. Figures 3(ac) show the x--plane positions of such a molecular enz semble with an initial Gaussian position distribution at the origin at dierent times. The spatial separation of molecules with dierent spin projections is clearly visible. By choosing a dierent value of 0 and 0 0 /, 12 13 23 we also obtain a spatial separation of molecules with different chirality, see Fig. 3(d-f). The separation is partial in the following sense: for our choice of parameters, righthanded molecules in the spin-up state are deected to nite values of x, whereas the other three components are not deected and their trajectories remain close to x = 0. By changing 0 0 , the role of left and right in 12 12 Fig. 3(a-f) is interchanged. In Fig. 4 we show the eective magnetic elds (i.e., the curl of the vector potentials) and scalar potentials leading to this behavior. Figure 4(a) shows the eective magnetic elds corresponding to all the subplots in Fig. 3 [the eective magnetic eld is the same in Figs. 3(a-c) and 3(d-f)]. For the situation in Fig. 3(a-c), the eects of the scalar potential (which is not shown) can be neglected: the magnetic elds are dominant and make the molecules in the spin-up state move along the x-direction (spin-down states along the x-direction). In Fig. 3(d-f) the scalar potentials are dominant (Fig. 4(b)) and will trap the molecules in the area around x = 0, except for the | R molecules that are deected. Stern-Gerlach experiments can also be used to obtain and measure superpositions of spin states. However, our

(a)

1110

*10

z/

(b)

320

z/

t

-200 -100 0 100

*10

200

310

10 0 -10

(c)

t

FIG. 4: (Color online) (a) Eective magnetic eld correspond2 ing to Fig. 3 (in units of k12 4 2 /2 ); (b) Eective scalar potential corresponding to Fig. 3(d-f).

z/

-200

-100

100

200

x/

L

1170

(d)

t *10

7

z/

R

R

200

400

600

360

z/

(e)

t

-400 -200 0 200 400

10

*10

600

z/

(f)

0 -10 -600

-400

-200

200

400

600

x/

FIG. 3: (Color online) The positions of an oriented molecular ensemble with an initial Gaussian position distribution 2 2 ((x, z)=(2r )1 exp[(x2 +z 2 )/r ] with r = 3) at dierent times. The positions x, z are in units of (the wavelength for the lower transition = 2/k12 = 2c/12 with c the optical velocity in vacuum; typically, 1 m). The following parameters are used: (a-c): 0 = 0 0 / 106 ; (d12 13 23 f): 0 = 0 0 / 104 (the detuning 1010 Hz is 12 13 23 large). Here, we assume 13 23 = 10, 12 = 7, x = 3, 0 0 . The molecular mass is taken to be 100 times the 13 23 proton mass.

in contrast to our conguration, the eect discussed in [6] cannot be used to distinguish and separate left- and right-handed molecules. Conclusion. In conclusion, we have studied the orbital eects of internal adiabatic transitions on the center-ofmass motion of oriented chiral molecules. We have shown that under the conditions described above, the center-ofmass motion of the molecules depends on both chirality and spin due to the optically induced gauge potentials and can be interpreted as a generalized Stern-Gerlach eect. This leads to the possibility of spatially separating molecules of dierent chiralities. This work was supported by the European Union under contract IST-3-015708-IP EuroSQIP, by the Swiss NSF, and the NCCR Nanoscience, and also by the NSFC and NFRPC of China.

eect described above does not work for superpositions of left- and right-handed chiral states (even if many studies about teleporting, preparating and measuring superpositions of chiral states [19] appeared recently), since this would require considering higher excited symmetric/antisymmetric states. We will leave this interesting question for future works. Although the protocol presented here is idealized since inter-molecular interactions are neglected, it provides a promising way to spatially separate molecules of dierent chiralities. A similar generalized Stern-Gerlach eect has been proposed for -type systems where the Rabi frequencies 12 between the two lower inner states vanish [6]. However, this eect is chirality-independent. Thus,

[1] D. Bohm, Quantum Theory (Prentice-Hall, Englewood Clis, NJ, 1951). [2] F. Wilczek and A. Zee, Phys. Rev. Lett. 52, 2111 (1984). [3] J. Moody et al., Phys. Rev. Lett. 56, 893 (1986). [4] C. P. Sun and M. L. Ge, Phys. Rev. D 41, 1349 (1990). [5] P. Zhang et al., Eur. Phys. J. D 36, 229 (2005). [6] S.-L. Zhu et al., Phys. Rev. Lett. 97, 240401 (2006). [7] X.-J. Liu et al., Phys. Rev. Lett. 98, 026602 (2007). [8] J. E. Hirsch, Phys. Rev. Lett. 83, 1834 (1999); S. Murakami et al., Science 301, 1348 (2003); S. Murakami et al., Phys. Rev. Lett. 93, 156804 (2004); J. Sinova et al., Phys. Rev. Lett. 92, 126603 (2004); Y. K. Kato et al., Science 306, 1910 (2004). [9] P. Krl and M. Shapiro, Phys. Rev. Lett. 87, 183002 a (2001). [10] P. Krl et al., Phys. Rev. Lett. 90, 033001 (2003). a [11] M. Shapiro, E. Frishman, and P. Brumer, Phys. Rev. Lett. 84, 1669 (2000). [12] Y.-X. Liu et al., Phys. Rev. Lett. 95, 087001 (2005). [13] P. Krl et al., Phys. Rev. A 72, 020303(R) (2005); Y. Li a et al., Phys. Rev. A 73, 043805 (2006); J. Q. You et al., quant-ph/0512145. [14] C. P. Sun et al., quant-ph/0506011. [15] H. Frhlich, Phys. Rev. 79, 845 (1950); S. Nakajima, o Adv. Phys. 4, 363 (1955). [16] J. Ruseckas et al., Phys. Rev. Lett. 95, 010404 (2005). [17] G. Juzeliunas and P. Ohberg, Phys. Rev. Lett. 93, 033602

5

(2004); G. Juzeliunas et al., Phys. Rev. A 73, 025602 (2006). [18] Alternatively, instead of the gravitational eld, we could use an initial velocity of the molecules in the direction z . [19] C. S. Maierle and R. A. Harris, J. Chem. Phys. 109, 3713 (1998); C. S. Maierle, D. A. Lidar, and R. A. Harris, Phys. Rev. Lett. 81, 5928 (1998); R. A. Harris and J. D. Walls, AIP Conference Proceedings 596, 186 (2001).

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