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Resonance Coalescence
Resonance Coalescence
When molecules are exposed to laser fields, their bound More recently, different manifestations of the EP phe-
states become metastable (the so-called resonances) which nomenon have been described in optics [8], in atomic
have a finite lifetime due to ionization and/or dissociation. physics [9,10], in electron-molecule collisions [11], super-
In the present Letter, we consider the photodissociation of conductors [12], quantum phase transitions in a system of
H2þ . The corresponding rates of decay or lifetimes @= interacting bosons [13], and electric field oscillations in
depend on the initial vibrational state and are associated microwave cavities [14], and in P T -symmetric wave-
with the imaginary part of the complex energy eigenvalues guides [15]. Varying the Hamiltonian parameters in an
E i=2 of the molecular Hamiltonian dressed by light. adiabatic way along a closed path which encircles the EP
These eigenvalues represent the poles of the scattering has been examined in a study of Hernández, Jáuregui, and
matrix [1–3]. The value of depends on the laser parame- Mondragón [16], who have shown that there is an inter-
ters (wavelength and intensity I). It might happen that for change between the two distinct resonance solutions which
very specific laser parameters two different resonances merge at the EP. This is a characteristic feature of an EP,
(each of them being issued from a different field-free interpreted mathematically as an effect of the multivalued-
vibrational state of H2þ ) coalesce. This special situation ness of a function of a complex variable detected whenever
cannot be adequately treated within the framework of the going around a branch point. To the best of our knowledge,
conventional Hermitian quantum mechanics (QM) where no theoretical or experimental work regarding EPs has so
all of the state vectors possess a real positive definite norm far been pursued in the context of laser driven photodisso-
and even the concept of a resonance is not well defined. ciation dynamics of molecules. It is the purpose of the
The coalescence of two different mutually orthogonal present work to demonstrate numerically the existence and
resonance states into a single self-orthogonal state can be physical implications of EPs for the case of laser induced
mathematically defined only within the framework of the photodissociation dynamics of H2þ . The Hamiltonian pa-
non-Hermitian formalism of QM, where complex energy rameters to be varied here are the intensity and frequency
eigenvalues appear and where one deals with complex of a linearly polarized laser light.
valued norms defined on the basis of the so-called c Let us briefly outline the theoretical formulation of the
product [4]. The points (, I) in parameter space where molecular photodissociation problem. We assume that the
self-orthogonality occurs are usually called exceptional laser field couples only the two electronic states X 2 þ
g and
points (EPs) [5,6]. In the present Letter, we will show A2 þ þ
u of H2 , denoted hereafter as jgi and jui, respectively.
that self-orthogonal resonance states do exist in the context The associated Hamiltonian is expressed as a 2-by-2 matrix
of molecular photodissociation and have important experi-
TR þ Vg ðRÞ dðRÞE 0 cosð!L tÞ
mentally observable consequences. Namely, we shall ex- H ðtÞ ¼ : (1)
ploit the self-orthogonality phenomenon to build a chirped dðRÞE 0 cosð!L tÞ TR þ Vu ðRÞ
laser pulse which operates a selective transfer from one Here R stands for the vibrational coordinate, and TR ¼
vibronic state of H2þ into another for those molecules
which have not dissociated during the process of interac- ½@2 =ð2H2þ Þðd2 =dR2 Þ is the usual vibrational kinetic
tion with the pulse. energy operator, with H2þ the reduced mass. The functions
Self-orthogonality phenomena in atomic physics have Vg;u ðRÞ represent the potential energy curves of the two
been analyzed theoretically a long time ago [7] for the case electronic states. The dipole matrix element between these
of the complex rotated Hamiltonian of the helium atom. two electronic states is denoted as dðRÞ. The standard
-5000
v=9
thus to photodissociation in the presence of the laser. For v=9
scattering matrix. The real part ReðEF Þ of a given complex 1000 v=10
determines the corresponding decay rate. Outgoing bound- 0 0.2 0.4 0.6 0 0.2 0.4 0.6
I (10 13 W/cm 2 )
ary conditions imply that the resonance wave functions are
not square integrable. To overcome this difficulty, we shall FIG. 1 (color online). Left column: Near coincidence of two
follow the well established approach of complex scaling resonance energies issued, respectively, from the field-free vibra-
transformations [2,3] which forces the resonance wave tional states v ¼ 8 and v ¼ 9 of the X2 þ þ
g state of H2 for the
functions to decay exponentially as R ! 1. After the 8–9 8–9
laser parameters EP ¼ 442:26 nm and IEP ¼ 0:3949
complex scaling transformation is implemented, the so- 1013 W=cm2 . Right column: The same for the case of v ¼ 9
called self-overlap of a given resonance solution and v ¼ 10 and 9EP–10 ¼ 401:14 nm and IEP 9–10
¼ 0:5130
F ðR; tÞ is evaluated as 13
10 W=cm . 2
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PRL 103, 123003 (2009) PHYSICAL REVIEW LETTERS 18 SEPTEMBER 2009
Re (E) (cm-1)
0
v=8 v=9 v=10 finds the molecule in its v ¼ 9 (or reciprocally v ¼ 8)
Im (E) (cm -1)
vibronic field-free state. Of course, this applies again
-500
only if not all molecules have dissociated during an adia-
batic passage along the loop. If a significant portion of
-1000
undissociated molecules is left after completion of the
-7000
460
-6500 -6000 -5500 -5000 -4500 -4000 contour, we have achieved a selective light induced transfer
between two specific molecular vibronic states. The third
contour drawn in Fig. 2 uses Imax ¼ 0:6 1013 W=cm2
440
EP(8,9)
λ (nm)
123003-3
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PRL 103, 123003 (2009) PHYSICAL REVIEW LETTERS 18 SEPTEMBER 2009
do not dissociate during the application of the adiabatically [9] O. Latinne, N. J. Kylstra, M. Dörr, J. Purvis, M. Terao-
chirped laser pulse), while the 8th to 9th transition is not Dunseath, C. J. Joachain, P. G. Burke, and C. J. Noble,
feasible. Owing to the multichannel character of the for- Phys. Rev. Lett. 74, 46 (1995).
malism, the observed coherent control scheme is expected [10] H. Cartarius, J. Main, and G. Wunner, Phys. Rev. Lett. 99,
173003 (2007).
to persist for other molecular species and with the intro-
[11] E. Narevicius and N. Moiseyev, Phys. Rev. Lett. 84, 1681
duction of rotational degrees of freedom. Other possible (2000).
signatures of exceptional points would be to examine, in [12] J. Rubinstein, P. Sternberg, and Q. Ma, Phys. Rev. Lett. 99,
the context of photodissociation, the zeros in absorption 167003 (2007).
line shapes resulting from the interference between over- [13] P. Cejnar, S. Heinze, and M. Macek, Phys. Rev. Lett. 99,
lapping resonances, as done by Shapiro [23,24]. An EP is 100601 (2007).
actually an extreme case of overlap. Such signatures have [14] C. Dembowski, H.-D. Gräf, H. L. Harney, A. Heine, W. D.
already been discussed in scattering processes for one- Heiss, H. Rehfeld, and A. Richter, Phys. Rev. Lett. 86, 787
dimensional model systems by Vanroose et al. [25] and (2001).
Hernández, Jáuregui, and Mondragón [26]. [15] S. Klaiman, U. Günther, and N. Moiseyev, Phys. Rev. Lett.
The authors gratefully acknowledge Professor Arne 101, 080402 (2008).
[16] E. Hernández, A. Jáuregui, and A. Mondragón, J. Phys. A
Keller, Dr. Ido Gilary, and Mr. Shachar Klaiman for fruitful
39, 10 087 (2006).
discussions. [17] O. Atabek, R. Lefebvre, and T. T. Nguyen-Dang, in
Handbook of Numerical Analysis, edited by C. Le Bris
(Elsevier, New York, 2003), Vol. X.
[18] A. F. Siegert, Phys. Rev. 56, 750 (1939).
*Also at U.F.R. de Physique Fondamentale et Appliquée, [19] M. Chrysos, O. Atabek, and R. Lefebvre, Phys. Rev. A 48,
Université Pierre et Marie Curie, 75321 Paris, France. 3845 (1993); 48, 3855 (1993).
[1] R. Taylor, Scattering Theory (Wiley, New York, 1972). [20] O. Atabek, R. Lefebvre, C. Lefebvre, and T. T. Nguyen-
[2] N. Moiseyev, Phys. Rep. 302, 212 (1998). Dang, Phys. Rev. A 77, 043413 (2008).
[3] W. P. Reinhardt, Annu. Rev. Phys. Chem. 33, 223 (1982). [21] F. V. Bunkin and I. I. Tugov, Phys. Rev. A 8, 601 (1973).
[4] N. Moiseyev, P. R. Certain, and F. Weinhold, Mol. Phys. [22] A. Fleischer and N. Moiseyev, Phys. Rev. A 72, 032103
36, 1613 (1978). (2005).
[5] T. Kato, Perturbation Theory of Linear Operators [23] M. Shapiro, J. Chem. Phys. 56, 2582 (1972).
(Springer, Berlin, 1966). [24] M. Shapiro, Phys. Rev. A 75, 013424 (2007).
[6] W. D. Heiss and H. L. Harney, Eur. Phys. J. D 17, 149 [25] W. Vanroose, P. Van Leuven, F. Arickz, and J.
(2001). Broeckhove, J. Phys. A 30, 5543 (1997).
[7] N. Moiseyev and S. Friedland, Phys. Rev. A 22, 618 [26] E. Hernández, A. Jáuregui, and A. Mondragón, J. Phys. A
(1980). 33, 4507 (2000).
[8] M. V. Berry, Czech. J. Phys. 54, 1039 (2004).
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