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T W^^ AD-779 887 MULTIPHOTON DETACHMENT OF NEGATIVE IONS N . M . Kroll , et a I Stanford Research Institute Prepared for: Defense Advanced Research Projects Agency March 1974 DISTRIBUTED BY: Kfül National Technical Information Service U. S. DbPARTMENT OF COMMERCE 5285 Port Royal Road, Springfield Va. 22151 i-v m* ^^ ^ ^

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■ UP T mma^m W^^

AD-779 887

MULTIPHOTON DETACHMENT OF NEGATIVE IONS

N . M . Kroll , et a I

Stanford Research Institute

Prepared for:

Defense Advanced Research Projects Agency

March 1974

DISTRIBUTED BY:

Kfül National Technical Information Service U. S. DbPARTMENT OF COMMERCE 5285 Port Royal Road, Springfield Va. 22151

i-v

_*< i i fc^i m* ^^■^ ^

y

Technical Report JSR-73-6

00 00 OS

^ MULTIPHOTON DETACHMENT OF NEGATIVE IONS

.Vcwo/> 1974

By: N M KROLL K M WATSOr,

Contract No DAHC15-73-C-0370 ARPA Order No 2504 Program Code No 3K10 Date of Contract; 2 April 1973 Contract Expiration Date 30 April 1974 Amount of Contract: $589,123

D D C ■

j üLJ

JUN 5 1974

J.

Approved or public release; distnbution unlimited.

Sponsored by

DEFENSE ADVANCED RESEARCH PROJECTS AGENCY Ar»"A ORDER NO. 2504

r

STANFORD RESEARCH INSTITUTE Menlo Park, California 94025 • U.S.A.

Rf-produced by

NATIONAL TECHNICAL INFORMATION SERVICE U S Department of Commerce

Springfield VA 22151

The views and conclusions contained in this document are those of the authors and should not be interpreted as necessarily representing the official policies, either expressed or implied, of the Defense Advanced Research Projects Agency or the U.S. Government

Copy No. .1.3..

33

^x. ^ j

^-r^T ■a ■^^^ ^^

^

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— REPORT DOCUMENTATION PAGE 1 REPORT NUMBER 2. GOVT ACCESSION NO

-L 4. TITLE (and Subtitle1

MULTI PHOTON DETACHMENT OF NEGATIVE IONS

READ INSTRUCTIONS BEFORE COMPLETING FORM

3 RECIPIENTS CATALOG NUMBER

5. TYPE OF REPORT & PERIOD COVERED

Technical Report JSR-73-6

7. AUTHOR!»)

N. M. Kroil K. M. Watson

9. PERFORMING ORGANIZATION NAME AND ADDRESS

Stanford Research Institute Menlo Park, California 94025

6 PERFORMING ORG REPORT NUMBER

SRI Project 3000 8 CONTRACT OR GRANT NUMBERIsl

Contract DAHC15-73-C-0370

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11 CONTROLLING OFFICE NAME AND ADDRESS

Defense Advanced Research Projects Agency 1400 Wilson Boulevard Arlington. Virginia 22209

14 MONITORING AGENCY NAME & ADDRESS (if dl«. from Controlling Office)

12 REPORT DATE

March 1974

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^L 15 SECURITY CLASS, (of thi» report!

UNCLASSIFIED

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18. SUPPLEMENTARY NOTES

Approved for Public Release; Distribution Unlimited.

19. KEY WORDS (Continue on reverte tide if necewary and identifV by block number)

Theoret ical Numerical

Multiphoton Electron Detachment Negative Ions

0 and 0

Intense Laser

'20. ABSTRACT (Continue on re«r,e tide if nece.«ry and .dentify by block lumber)

A theory is presented to describe multiphoton detachment of negative ions by Intense laser beams. The detachment rate is expressed in terms of the single-photon detachment rate. Numerical results are presented for detachment of electrons from 0" and Og. Critical comments are given concerning some theories of multiphoton ionization.

DD.2r»1473 EDITION OF 1 NOV 65 IS OBSOLETE

» SECURITY CLASSIFICATION OF THIS PAGE (When Data Entered)

- '■ * • IM M* ^^^ «6

i

r-^7 7

CONTENTS

DD Form 1473

I ABSTRACT I

LIST OF ILLUSTRATIONS iv

I INTRODUCTION !

11 FORMULATION 3

III PiE QUASISTATIC APPROXIMATION 8

IV STUDY OF THE QUASISTATIC APPROXIMATION ü

V DETACHMENT OF 0 20

VI DETACHMENT OF o" 2Ö

ACKNOWLEDGMENT 28

REFERENCES 29

PNCÄ W Wank

in

ir I I fcW — - ■*

W I UP T ^

ILLUSTRATIONS

The Fractionil Error in the Quasistatic Approximation

[Functions (62) and (63)] Shown as a Function of the

Final Electron Energy for 5-, 10-, and 20-Photon

Detachment of 0

Contour of Ii tegration for the Integral (68), Showing

the Two Branch Points u^ and the Two Saddle Points u . . . . b s

The Detachment Rate (73) for 0 Shown as a Function of the Laser-Beam Power Flux

The Detachment Rate for 0 Shown as a Function of Laser-Beam Power for Wavelengths oi 10.6 and 5.5 urn

19

23

2\

27

Iv

^X. ■ —

^

INTRODUCTION

I

The intense electromagnetic fields obtainable in laser beams can

induce multiphoton transitions in atoms and molecules with significant *

probabilities. A variety of such transitions have been observed.

Also, a number of theoretical studies of these processes have been

published. The simplest of these are essentially dimensional analyses3

and are very crude, but do provide useful scaling relations in the weak

field limit.

The most straightforward of the calculations of multiphoton tran-

sitions use perturbation theory.4 These calculations are, unfortunately,

of great numerical complexity and are consequently ordinarily carried out

with such gross approximations that the results are probably not much

more accurate than are those of the above-mentioned dimensional analyses.

The perturbation calculations, of course, fail to describe transitions

.in very strong fields.

A somewhat intuitive and partly phenomenological calculation by

Keld"sh5 takes account of distortion of the atom or molecule by the

intense fields and also of transitions taking place through a nearly

resonant intermediate state. Keldysh's theory is not restricted to the

Several reviews of multiphoton processes are available in the

literature.1"! See also R. A. Fox ot al.2

References are listed at the end of the report.

^^X. ^

^■^^^^

^

weak field limit, as is perturlation theory, and at the same time

provides rather simple expressions for the transition rates.

A technique developed from first principles and not restricted to

perturbation theory has been published by Reiss.6

The specific process studied in this report is the detachment of

an electron from a negative ion by multiphoton absorption. It will be

assumed that the photon energy hcu 1B significantly less than the detach-

ment potential I. Our method i.. not applicable *or evaluation of ioni-

zation of neutral atoms or molecules unless the Coulomb potential in

2 the final state is screened at distances less than (hio/e ). jli.dy of

the failure of our theory for ionization processes demonstrates what

appear to be significant inaccuracies in the theories of both Kelaysh

and Reiss.

Certain approxiuations will be made. These are:

(1) The electromagnetic field of the laser is treated classically

and is assumed to vary sinusoidally with the frequency ou.

This implies that the beam Is intense enough that quantum

fluctuations of th' E and B fields are negligible and also

that th',- beam cohvrjnce time is long compared with that for

the transition tu occur.

(2) It ii assumed thnt only electric dipole transitions need be

considered, that the photon wavelength is very large compared

wlt'i atomic dimensions, and that relativistic corrections for

electronic motion may be neglected.

(3) We shall assume that only a single electron orbital is involved

in the transition. That is, we shall treat the problem as

thovgh it were the case of a single electron moving in a

specified binding potential. We thus avoid the complexity

of many-body interactions.

'- * ■ ~*- Mta ^^am

^

II FORMULATION

Let h 2 h(p,x) represpnt the Hamiltonian of the atom (or molecule).

Here we suppress the explicit dependence on all coordinates except the

momentum p and space coordinate x of the "active" electron. In the

presence of the electromagnetic field the full Hamiltonian is

H ■ h(p - a, x) (1)

where -» e -* a s - A

c (2)

with A the vector potential of the electromagnetic field. We shall

treat the vector potential as classical, writing it in the form

4S cos (u)t + 0 ) o

(3)

V

where uu is the angular frequency of ehe field and 0 is a censtant.

We note that

-a = eE = eE sin(u)t + 0 ) o o

A 2-» eE = uu a

Here E is the electric-field intensity.

(4)

—————

^^X.

-^■w^"^^"^-

^

The Hamiltonian, Eq. (1), may be written as

H = H + A o

(5)

with

A = p • a/m

H = h + — o 2m

(6)

The quantity H represents the "unnerturbed" Hamiltonian, and A the part o

that leads to transitions. It would evidently not be sensible to treat

the term a /2m as an interaction, since this C-number commutes with the

electron variables.

The initial state of the ion (or atom) with the active electron

bound to it is 0 , where a

h 0 = W 0 a a a

The solution of the time-dependent Schrödinger equation

H 0 = i 0 o

corresponding to the initial state, is then

-iW t -ivCt) 0(t) = 0 e a e

(7)

(8)

(9)

where

v(t) = f ait') ^mdt' (10)

-u I I «Ji ^

^

The final state, when the electron is out of range of the potential of

f the residual ion (or atom), is 0 . This satisfies the Schrodinger

equation

-» -♦ 2 f 'f [(p - a) /2m] 0 = i0 , (ID

or

f /o -3/2 ik-x -iv (t) 0 = (2n) e e k

(12)

where t

Yk(t) =f |[k - ^(t')]2^ jdt' (13)

The complete process is described by the wave function \Kt) that satis-

fies the full Schrodinger equation

H\|) = iii (34)

with the boundary condition that

lia iKt) = 0 (t) t-W-oo

(15)

If we imagine the electromagnetic field to be turned on very slowly

in the remote past and off very slowly in the remote future, the S-matrix

for the transition is

S = Xim U(t), 0(t))

t-*+<»

(16)

* 7 See, for example, M. L. Goldberger and K. M. Watson. Note that the

outgoing-plane-wave boundary condition is used in Eq. (16).

■—

_U A ** M fc

Ill ■

^

Following standard wave-packet arguments, we have

00

-i j dt [-1 A (M)]

-1 / dt [(ii,0) - (^,10)]

-i I dt(ili(t),A(t)0(t)) (17)

I

A perhaps more useful form for the S-matrix is obtained on making

the gauge transformation

| = e ix«a

y (18)

This transforms Eq. (14) into the form

(h + r>j - M (19)

where

F(t) = -ex . E(t) (20)

The S-matrix in this representation is

3 = -i

00

/ dt ^(t), P(t)|Ct>j (21)

Here

J(t) = cp e a a

v22)

•__

_fci. I 1 fc^ i ■ ^—**--!

=^■«7 ^

The total rate of ionizatlon is obtained from the expression

R-| \ k

T 2

[ dt(i|i( A0)

T 2

(23)

or

1 R = ^ r -» T

k

I 2

I dt(Y, F$) (24)

Here T is some long time interval, chosen lar.je enough that R is

independent of T.

The expressions (21) and (24) were used by KeldyshB in his dis-

cussion of multiphoton ionization.

-

^r

III THE QUASI STATIC APPROXIMATION

In this section we discuss a low-frequency approximation, assuming

that

•heu « I = -W a a

(25)

The condition (25) was assumed also by Reiss6 and by Keidysh.5

The limit (25) suggests that we begin with solutions to the eigen-

value equation

Hx = **. -* k -* k k

(26)

where em -3/2 ik-x (2IT) e

k jtimx-»ai

(27)

consistent with Eq. (15). The transformation

± ix-a + r = e 0 (28)

converts Eq. (26) into the form

± ± h0 = W 0

-♦ -* -* K k K

^^ - ^mrn^J

T ^r

The boundary condition (27) leads us to conclude that

t. k - a

W = K /2m = c (29)

so the 0 satisfy the Lippmann-Schwlnger equation

K

h0 = e0 t KK

(30)

If a can be treated as slowly varying, one might then expect that

-IV (t) ^ =?; X e k

^0 e-i\(t)

(31)

(32)

would provide approxim re solutions to the time-dependent Schrbdinger

equation. The conditions under which Eqs. (31) and (32) are valid

approximations will be studied in the next section.

If, for the moment, we assume that Eqs, (31) anu (32) are valid,

the expression (21) takes a rather simple form. We have

S =

OS

-i Lei[Iat+\(t)] (0-.e^0a) • E sin(u)t + 0 ) . (33)

o o

X

:v ^^ -

■^r ^r

Now -♦ = /0 , ex0 \ d U V

is just the dipole matrix element for the single-photon photoelectric

process. Thus, knowledge of this matrix element will enable one to

evaluate the multiphoton transition rate when Eq. (32) is valid.

For evaluation of the expression (33) the Fourier series expansion

of Keldysh is conven ont. First we define

2_

(U

S = o

- — / dt sin(u)t + 0 )exp |i[l r + Y, (t)]| 2n j o L a k J

(0 , ex0 \ • E

U 7 0 (34)

to obtain

2 2 e E

^ 6 ll + e + 1 - +' I v=-oo \ 4muü

(35)

Equations (34) and (35) were used by Keldysh, but with 0^ replaced K

by a plane wave:

-" ,0 x-3/2 ^'X 0 « (2rt) e K

(36)

10

•mmmm^^mmm

-

■^r ^r

IV STUDY OF THE QUASISTATIC APPROXIMATION

In this section we study some conditions under which the quasi^tatic

expressions (31) and (32) might be expected to be valid. For this pur-

pose wc write

-IV (t) ♦ = X e k (37)

and require that this be an exact solution of Eq. (14). On noting the

relations (4), we see that the general form of X is

k

X = e 0 (x, a, E) (38)

Indeed, substitution into Eq. (14) gives us the following equation for

0 t

h - ex-E + eE'(- V ) - e I 0

L V1 tl KJ t

[i BL'V 0 - eE

f t a Kj

(39)

First, let us consider the strong field limit and assurae that |al

can be treated as large. Then we expect the Born approx.mation to be 2

valid with h replaced by p /2m.

11

\ —

^r ^r

In this case

,„ -3/2 iK'x 0 ■ (2it) e -» K

(40)

is an exact solution of the modifitd Eq. (39) and the adiabatic approxi-

mation is valid. Equation (40), substituted into Eq. (34), leads just

to the expression used by Keldybh.

-» The above argument is not rigorous, since a is /arying sinusoidally

and must pass through zero. It does make it plausible, however, that

Eq. (40) can represent a fair approximation when (e£ /w) is large. This

is consistent with the observation of Keldysh that .n this limit (and

for uj-» 0) Eqs. (40) and (35) lead to Oppenhelmer' s' ?xpression (to within

a numerical factor) for ionizatlon of a neutral atom :• a static electric

field.

We next use Eq. (39) to study the adiabatic approximation in the

weak field limit—that is,

la| « k

—and of course continuing to assume condition (25). To do this we make

an eikonal approximation for 0 , writing

K

0 ~ e t

ir(x)

r = K

00

- I [Q(x') - K ] ds (x') (42)

12

ii ii >^i ■^=__^^k.

■^r ^

Since e « I , we take the eikonal trajectory to be a straight line k a

falling into the force center. This we take to be a static potential

[ -V(x)]. The quantity Q in Eq. (42) is taken to be the positive

root of

-*.-*. -* -* ,-» 2 2 Q = K + 2mV + eE'L^x) + a-L (x) (43)

where L and L are functions to be determined. To ensure convergence 1 2 -1

of Eq. (42), it is assumed that V (x) decreases faster than x as x-*».

Thus, if V is a Coulomb potential, we assume it to be screened at large

d.'JUnces. The quasistatic approximation is valid when L and L may be

neglected in Eq. (43). When a = 0, Q becomes

Q = |^k ' + 2mV (x)J 1/2

(44)

If we let the eikonal trajectory lie along the Z-axis of a rectangular

coordinate system, then Q = Q(Z) and Q = Q (Z) are functions of Z only.

Then

Q (Z) = kll + V (Z)/V (Zo)J 1/2

(45)

where

V(Z ) s «. o k

(46)

13

. :v ^ - -

^r ^^^^^^^

^

lo first order In a and E we obtain

T = T - a'x - e^ o

00

/(2Q ) o

-» - a

"00

/ LZ

L dZ,/(2Q ) - P 2 o a

(47)

where T is the function f for a = E = 0 (hence, K = k) and o

■ \ ] «, - /

k) dz' = k / (k/Q - 1) dz' = kP . (48) o a

Substitution of Eq. (42) into Eq. (39), with the standard WKB

approximation of neglecting gradients of Q, provides us with the coupled

equations (valid to first order in a and E)

cr

. /(2m) = P - / L /(2Q ) dZ7 1 * J 2 o

L /2m = u) 2

00

(2Q ) dZ7 o

(49)

-» -» -♦ -♦ where L = k L , L = k L . Use of these relations lets us re-express

Eq. (47) as

r = r - a-x + a'L /(2m) - eE'L /(lav ) o 1 2

(50)

14

-u i_^ - *- - •

^7 ^

The quasistatic approximation is seen to be valid vhen

L ^ 0, L /(2m) 2: P 2 1 a

(51)

To integrate Eq. (49) we introduce the new variable;

v(Z) =

z

/(k/Q )dZ//a o

(52)

Then

— [L /(2m)l - -aflL. dv L 2 J 1

/(2m)

where

± (L /(2m)l = —^ + a L /(2k) dv I 1 J dv o 2

Q H mum /k = Ha)/ 2 (ek * )

(53)

(54)

The quantity (48) may be expressed in terms of v. We first define

Then

P(Z) = a v(Z) -Z o

P (Z) = P(») - P(Z) a

Equation (53) may be integrated in the form

L /(2m) = P - P 1 a

L /(2m) = (tu/n)

oo

/ V

m

I

sin [iKv' - v)]P (v^dv a

1 - cos

15

(55)

(56)

[fUv' - v^jr^'Mv' . (57)

/

A. -^

^7 ^■^»—^i

^

Here d2P

r(v) = (58) dv

Alternatively, we can express L as

L /(.2m) = fl

00

sinQKv' - v)] TCv^dv' (59)

We note from the conditions (51) that the quasistatic approximation

will be valid in the limit fi -* 0 if the integral

00

/ P (v^dv'

is finite for all v and if the potential V is not more singular than the

Coulomb potential at Z = 0.

We first study the case of a screened Coulomb potential (that is,

a final ion state). Let us as me that the potential is screened at a

distance R and take [see Eq. (46)]

Z = e /e, O k

For Z « Z (and « R), we obtain o

(60)

16 i

„f

^^ - ^*m

^^N ^

L (Z)/(2ni) = L (0)/(2m) + Z + . .

L (Z)/(2mu)) = L (0)/(2mu)) 2 ^

- - (Z/a )3/2 (a /Z )1/2 fl L (0)/(2in) 3D O O 1

+ . . . (61)

The linear Z-term in J. corresponds to the Reiss factor exp(i a'x).

The L (0) and L (0) terms (independent of the space coordinate) arise

in satisfying the boundary condition at |x| = «. These are time-dependent,

so they will contribute to S [Eq. (34)]. Indeed, since Ll(0)/2m » ao,

we see no reason to neglect these terms.

When the screening radius is R « Z (but »a ), we can evaluate

the relative error in the quasistatic approximation from

■■>-\h (0)/(2m) - P (0)| /P (0) a J a

« (R/a )3(WRy)2/(12) . (62)

When this quantity is sufficiently small compared to unity, we expect

the quasistatic approximation to be valid.

For R » E the quasistatic approximation does not appear to be o

valid. Numeri'-al evaluation of Eq. (62) gave values of gi and

g = II (0)/[2mu) P (0)]| 2 I 2 a I

(63)

to be about unity for a wide range of parameters. Furthermore, an

estimate of the second-order terms in a and E, omitted from Eq. (50),

indicated a contribution comparable to the first-order terms when So

[Eq. (34)] is evaluated.

17

^-N ^

We conclude, then, that for a final ionic state, with rcreening

distance R » Z , we are not able to evaluate multiphoton ionization o

rates. Since we have found what appear to be large corrections in "he

expressions used by Keldysh5 and Reiss,6 our confidence is not great

in tie accuracy of their results.

We are able to draw a more optimistic conclusion for detachment

of an electron from a negative ion when the residual molecule does not

have P. significant permanent electric dipole moment. In this ase the

potential in the final state has the asymptotic form

-V(r) = a e / P /

2 / 4 (2r ) (64)

r -> oD

where 0 is the polarizability. P

3 For photodetachment of 0 wr h.ive a <** 5.29 and I = 1.46 eV. r p ft

Equation (67) should be numerically evaluated for a potential with the

asymptotic term (64) and for small r modified to remove the singularity

at r = 0. The error functions g and g are shown in Figure 1. The

curves are labeled by N, the )east number of photons required for

detachment, and are given as functions of e = N lur - I . As anti-

cipated, we see that for large N, and an e not too snail, both g^^ and

g become small, as required for the validity of the quaslstatic

approximation.

18

v ^MW* m^mm

^

I

— oft;

/

U

'

„ z s? o S t — o * •o ? ^

— f^ ^ £ D E

z a c ^ o o . ♦= U O K 1^ i

U. i" 3

£* ' 2 o ,„ <>£

ibfl X (E o "J QC Z a. ui a. <S ü QC

C o

n c

< a

< Cl

tr 0i 0 z •-

itc ^ o o

z u. o

OC -, ^

UJ o t- 1 I UJ I- w Q

oc

a

c I IQ

0 'U0UU3 IVNOIlOVUd

19

^^ a— m*

^x ^

V DETACHMENT OF 0

We now use the expression (34) to eval..ate the m"ltipho1on detach-

ment rate of 0 in the weak field limit. The single photon detachment

rate has been studied experimentally by Branscomb et al.9 Theoretica1

studies have been made by Brueckner and Klein10 and by Gillespie.11

Since the attached electron is in a p-orbital state the transition will

take place to a state of zero angular momentum if the electron energy

is sufficiently low. We thus use condition (25) to write11

Al" , e x 0 ^ E ft f'VlO \t 7 0 CE (65)

where C is a constarc and f is the Jost funrtio' ,hich we write in the

effective-range approximation as

f" (-K) = (K + ia)/(K + ib) (66)

Here a and b are constants related to the scattering length and effective

range lor plectron scattering by a neutral oxygen atom.

See, for example, Ref. 7, p. 540.

T. F. O'Malley et al.la have shown that for a potential having the

asymptotic form (64) the effective range expansion is modified. For

the very low electron energies of interest to us this modification

is not significant.

20

.X. i^te

■^ y

Following Keldysh,5 we take 0 = — and introduce the variable o 2

u= sin jut in Eq. (34). We shall assume that the electromagnetic field

is weak in the sense that

(eE Au) « k o

(67)

We rewrite (34) in the form

S = - (2Tt) o

-1 /du iQ(k,u) L/H^T e J CE (68)

Here the cloi. contour encloses the points u = -1, 1 and lies within iO

any other singularities of e /f.

in the weak field limit we can deform the contour so that every-

where on it |u| » 1. An elementary evaluation gives us, then,

iQ JJ 2 r -* -* 2 T —N e = (i/2) exp(- ßu /4) exp[-ek'E u/(müü )Ju , |u| » 1 . (69)

Here

"[.. 2 2 2 •i- ek + e Eo/(1.iuj )| (tn ) )1 /(hüü)

is, according to Eq. (35), the number of photons required to detach f 2 2 2 1

the excess electron, and 0 = Ie E /(muu )| /(-hu)).

As Keldysh observed,5 Eq. (69) has two saddle poiitts at the roots

I + — K = 0 a 2m (70)

21

-

■^7 m*^^ 7

These correspond to

u fe tiv s ■ ^"yp^r /(eE ) (71)

As also observed by Keldysh, the expression (65) has poles at the

positions defined by (70). The quantity C. in Bq. (65). which is

really K-dependent, has poles at the same positions ii

Keldysh used the Born approximation, so in his expressions, f - 1.

He was thus able to evaluate (68) keeping only the contribution from

the saddle points at u 3r tiV.

-1 We cannot use the Keldysh approximation because f (-K) has branch

points at

u = u)(-k|| ±ikx)/(eE ) (72)

where k,, is the component of k parallel to |, and ^ is the component

of iT perpendicular to t^ Since |«J « juj our integral (68) will

receive its principal contribution from the vicinity of the branch

points. The contour of integration used is shown in Figure 2.

Evaluation of (68) is straightforward when N is large. The rate

of detachment is, final!:, in the limit of large N:

R = 2« f\b(l + e + e2E 2/(4mu)2) - Nhu)) |s J \ a k o /

2T 3 2QN Ry

X U(2e /hiu) eE /(2ku)) I eE /(2ku))

2N (73)

Equation (71) would be exact if ^ were zero. For nonvanishing k the

actual saddle pcints are displaced slightly from the position ± i Y.

22

I ■H

^^X. m* ^m

^"■^^» -N

^«31^^ W

FIGURE 2 CONTOUR OF INTEGRATION FOR THE INTEGRAL (68), SHOWING THE TWO BRANCH POINTS ub AND THE TWO SADDLE POINTS us. Branch lines are Indicated between u = -1 and +1 and from ±ub to ±us.

In tie lower version of this equation, k Is evaluated when the

argument of the 6-function vanishes, or Is the fine-structure constant,

and R Is the Rydberg constant. We have expressed R In terms of the

cross section a(k) for detachment by a single photon of energy

•hu) = I + e . Finally, 1 a k

V(x) =

x. 2n xcos 6 2Ä „

sin 9 dG (74)

23

_u I I fc^

^r wm^m ^

The ionlzation rate (73) is illustrated in Figure 3 as a function 2

of laser power density [expressed in watts/cm ] for several values of

the photon energy Iwu using the experimental values of a from Ref. 9.

We note that our result (73) is substantially different than that which

would be obtained from the Keldysh evaluation using the Born approxima-

tion.

POWER FLUX—W/cnT

FIGURE 3 THE DETACHMENT RATE (73) FOR 0" SHOWN AS A FUNCTION OF THE LASER-BEAM POWER FLUX. The curves are labeled by the photon energy in electron volts.

24

if ii a^i ^ ^^^m

—■N 7

I

It is interesting to observe that for large photon numbers the

cross section (73) is considerably enhanced for electrons near threshold,

Our weak field approximation (67) fails for very low electron energies,

however, and the apparent divergence of Eq. (73) at k = 0 is due to the

failure of this approximation.

25

1

ii ii >fci «* —j

F' i Ui "T 7

VI DETACHMENT OF 0

Cross sections for photodetachment of 0 have been published by

Burch et al.13 The detachment energy is I = 0.44 eV and the electronic a

2 configuration is a state. An electric-dipole transition cannot

g 2

take place to a final S-state for the H state. Geltmann14 has dis- g

cussed the implications of this for the near-threshold dependence of

the single-photon detachment cross section.

A theory of final-state enhancement does not seem to have been

given for nonspherical potentials. Until such a theory is available,

we shall use Eq. (73) with an appropriate shift of parameters. For

a (k) we shall take the experimental value of Burch et al.1 This is

admittedly not a rigorous theory. If, however, the dipole matrix

element has the branch points (72) as closest to the origin in the

fi-plane, the ionization rate is rather insensitive to other details

of the matrix element.

The resulting ionization rate as a function of laser power is

shown in Figure 4 for 10.6-am radiation.

v

' I "^ «M^ai

^

10' 10'

POWER FLUX — \Nlcw

KT 10' 2

FIGURE 4 THE DETACHMENT RATE FOR Oj SHOWN AS A FUNCTION OF LASER-BEAM POWER FOR WAVELENGTHS OF 10.6 AND 5.5 ßw

27

ii « » >^i ■ j

^^^^■^

^

ACKNOWLEDGMENT

The autho -s would like to thank Dr. Forrest Gilmore for a discussion

of the detachment of 0 and 0 .

28

X V

.^.^——-^

^^^

^

ElEFERENCES

1.

2.

3.

4.

5.

6.

7.

8.

9.

10.

11.

12.

13.

14.

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29

^^M