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Tamar Seideman- Current-driven dynamics in quantum electronics

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Tamar Seideman- Current-driven dynamics in quantum electronics

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journal of modern optics 2003, vol. 50, no. 15–17, 2393–2410

Current-driven dynamics in quantum electronics

TAMAR SEIDEMAN

Department of Chemistry, Northwestern University 2145 Sheridan Road, Evanston, Illinois 60208-3113, USA; e-mail: seideman@chem.northwestern.edu

( Received 12 March 2003; revision received 22 April 2003 )

Abstract. We suggest that inelastic electron tunnelling via molecular-scale electronics can induce a variety of fascinating dynamic processes in the molecular moiety. These include vibration, rotation, intermode energy ﬂow and reaction. Potential applications of current-induced dynamics in molecular- scale devices range from new forms of molecular machines and approaches to enhancing the conductivity of molecular wires, to new directions in nanochem- istry and nanolithography. Understanding the molecular properties that encourage current-triggered dynamics is relevant also to the design of devices that would be guaranteed to remain stable under current. We discuss the qualitative physics underlying current-driven dynamics, brieﬂy sketch a theory developed to explore these dynamics, describe a few examples from recent and ongoing numerical work and note avenues for future research.

1. Introduction

Considerable theoretical eﬀort has been devoted in recent years to the problem

of molecular-scale electronics. This research [1–17] has been fuelled by the

fascinating physics of conductance at the molecular level, by the anticipation for technological applications and by the development of experimental techniques to produce and characterize molecular-scale electronics [18–36]. Reviews of the theoretical and experimental aspects are given in [17] and [21] respectively.

A recent special issue on transport in molecular wires [37] provides a useful

up-to-date overview of this exciting ﬁeld. The combination of theoretical and numerical work in this area has yielded substantial insight into the response of the

conductivity to several general attributes [2–8], as well as quantitative predictions

of the conductance of a variety of speciﬁc systems [10–15].

A problem of signiﬁcant fundamental interest, which may also carry practical beneﬁt and which is only starting to be explored, is the eﬀect of the current on the molecule. Recent theoretical work [38], supported by indirect experimental evidence, suggests that inelastic tunnelling via molecular-scale devices can induce a variety of dynamic processes in molecular heterojunctions. These include

vibration, rotation, intermode energy ﬂow and reaction. The mechanism through which a tunnelling current at the mild conditions typical of molecular electronics research can trigger large-amplitude motion of a massive molecular backbone is simple and general. For applications such as molecular wires, favourable candidates are molecules that oﬀer resonances in energetically accessible regimes. Resonance-mediated conductance is eﬃcient

Journal of Modern Optics ISSN 0950–0340 print/ISSN 1362–3044 online # 2003 Taylor & Francis Ltd http://www.tandf.co.uk/journals DOI: 10.1080/0950034034032000120876

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T. Seideman

and at most weakly distance dependent. By contrast, direct tunnelling falls exponentially with increasing distance. Resonance conductance is often inelastic. Provided that the initial and resonant electronic states are displaced in equi- librium, the system evolves during the resonance lifetime. Upon electronic relaxation the molecule carries internal excitation which may suﬃce to trigger chemical dynamics before relaxing to the initial vibrational state [38]. Current-triggered dynamics in nanosystems carries potential implications and applications in several ﬁelds.

(i) New forms of molecular machines. The area of artiﬁcial molecular machines [39] has been evolving rapidly for nearly two decades, leading to laboratory-made turnstiles, shuttles; switches and rotors, driven by light, chemistry or electrochemistry. On the one hand, this work points to a host of potential technological applications [39]. On the other hand, it reveals the need for new forms of molecular machines, which could be addressed individually, thus eliminating the ensemble average that is inherent to the solution phase. Current-triggered dynamics in molecular heterojunctions could make a route to that end. We envisage using resonant inelastic current to deposit energy selectively into a given mode and hence to induce directed motion of the molecular component. (ii) Dynamic modiﬁcation of the conductivity of molecular wires. Often in

molecular wires the conductivity depends sensitively on the structure of the molecule [22]. An example is the biphenyl family, where the conductivity changes by over an order of magnitude as the torsion angle between the rings varies between zero and p /2. In these systems, torsion may be expected to ensue resonance tunnelling since the ionic states of biphenyl diﬀer substantially from the ground neutral state in equilibrium conﬁguration, speciﬁcally along the torsion angle. Current-triggered large-amplitude vibration may likewise modify the conductivity of wires. An experimental study of electron transfer from a metal surface to a molecule [40] found the electron transfer probability to be greatly enhanced by excitation of the molecule to high vibrational levels. Clearly, one can envisage systems where molecular motion inhibits the conduc- tivity, because the equilibrium is ideally conﬁgured for electron transfer to take place.

(iii) Nanochemistry. An intriguing possibility is that of using a scanning tunnelling microscope tip to induce surface reactions that do not occur spontaneously and to study them on a single-molecule, site-speciﬁc level. One class of systems of interest is the reactions of the common gas sources used for thin-ﬁlm growth on, and doping of, Si by chemical vapour deposition (NH _{3} for N, PH _{3} for P, and AsH _{3} for As, for instance). The thermal reactions currently used by advanced growth and doping tech- nologies are not ideal to that end, as is evident from the broad disparity between observations of diﬀerent laboratories [41] and from the variety of

undesired eﬀects reported [42]. The current-triggered approach may introduce an opportunity of controlling the outcome.

(iv)

Design criteria. Current-induced dynamics in molecular devices may have undesired consequences. In extreme cases they may lead to failure.

Current-driven dynamics in quantum electronics

2395

The design of current-immune devices relies on understanding the molecular properties that encourage current-triggered dynamics. (v) Opportunities in molecule-scale lithography. Nanolithography based on current-induced desorption of H atoms from Si(100) is an established ﬁeld with a variety of applications [43–47]. Organic molecules may oﬀer advantages. In the adsorbed state conjugated organics support low-energy resonances (lying close to the Fermi level), corresponding to much lower voltages than those used for H desorption from silicon; hence smaller tip– surface separations and improved resolution. Further, as discussed in [48], the properties of organic adsorbates can be tuned via functional group substitution, providing a means of control over the process.

In the next section, we outline a recently developed theory of current-driven dynamics in molecular devices. Section 3 describes several applications and the ﬁnal section concludes with an outlook to future research.

2. Theory and interpretation

We consider nuclear dynamics that are triggered by an inelastic resonance- mediated tunnelling event. In the tip–adsorbate–substrate environment, this would be a surface reaction induced by electron transfer from the tip to the surface or vice versa via an adsorbate-derived resonance. In the molecular wire environment, we envisage directed motion of the molecular moiety, induced by tunnelling from one electrode to the other via a resonance of the molecule þ electrodes Hamiltonian, as modiﬁed by the bias voltage. Formally the two prob-

lems are equivalent and can be studied within the same theoretical framework. Numerically, however, they diﬀer substantially, as outlined below. The complete Hamiltonian is written as

ð1Þ

where H _{e} describes the electronic dynamics and allows for hopping of electrons between the two electrodes via the adsorbate orbital, H _{N} is a system-speciﬁc nuclear Hamiltonian and H _{e}_{–}_{N} is the non-adiabatic interaction coupling the electronic and vibrational motions. It is convenient to expand the Hamiltonian in eigenstates of H _{e} , such that coupling between the extended electronic states of the two electrodes and the discrete state localized on the adsorbate is taken into account non-perturbatively. In this representation,

H ¼ H _{e} þ H _{N} þ H _{e} _{} _{N} ,

H e ¼ X

_{} c

y

c _{} þ ^{X} _{} c

y

c _{} ,

ð2Þ

where j i and j i are stationary electronic states on the two electrodes and _{} and _{} , are the corresponding energies. The coupling is written in the H _{e} representa- tion as,

H _{e} _{} _{N} ¼ h _{N} ðQÞ ^{X} ðh jr i h rj i c

;

y

c _{} h n _{r} iÞ,

ð3Þ

Equation (3) adapts the coupling term used in several early studies of vibrational excitation of a linearly coupled harmonic oscillator to the problem considered here [49].

2396

T. Seideman

where h _{N} (Q) is a function of the nuclear coordinates Q, jri denotes the resonant

orbital and hn _{r} i is

Assuming that the non-adiabatic interaction can be described within ﬁrst-order perturbation theory, we express the reaction rate w as

its equilibrium occupancy.

w ¼ 2 ^{2}^{p}

~

X

,

X

v

f _{i} ð _{} Þ½1 f _{f} ð _{} Þ jh v _{} , jH _{e} _{} _{N} j v _{0} , ij ^{2} ð _{} _{} Þ,

ð4Þ

where jv _{0} , i¼jv _{0} ij i, jv _{} , i¼jv _{} ij i, jv _{0} i is the initial vibrational state, a bound eigenstate of the nuclear Hamiltonian, and jv _{} i is a ﬁnal, bound or free eigenstate of the same Hamiltonian. We denote by the energy transferred from electronic into vibrational modes, ¼ _{} _{} , and the subscript to v _{} serves as a reminder that the energy of the ﬁnal state is restricted through energy conservation to above the initial state energy. In equation (4), v _{0} denotes collectively the set of quantum indices specifying the parent state. In the case of a bound–bound process in the nuclear mode (such as intermode energy ﬂow, rotational or vibrational excitation or a surface exchange reaction), v _{} has a similar signiﬁcance. In the case of a bound–free reaction in the nuclear mode (such as a desorption or a dissociation), v _{} denotes the scattering energy and the quantum indices specifying the internal state of the free product. In the latter case, the v _{} summation in equation (4) implies summation over the discrete indices and integration over the energy. The f _{i}_{(}_{f}_{)} (E) in equation (4) are Fermi–Dirac distribution functions. The assumption of Q-independence of H _{e} allows us to reduce equation (4) to a form that provides better insight and is substantially easier to handle numerically. To that end we ﬁrst separate the vibronic matrix element in equation (4) into interdependent electronic and nuclear factors and introduce a complete set of eigenstates of the ground nuclear Hamiltonian

I ¼ ^{X} jv i h v j þ ^{X} ð d j n ^{} ih n ^{} j,

v

n

ð5Þ

where jvi are bound and j n ^{} i are incoming wave scattering states of H _{N} . The collective index v denotes the bound-state vibrational indices and n speciﬁes the internal quantum numbers of the free state. With equations (3) and (5), the transition matrix element in equation (4) assumes the form

h v _{} , jH _{e} _{} _{N} j v _{0}_{,} i¼h j rih rj ih v _{} j ^{X} jv ih v j þ ^{X} ð d j n ^{} ih n ^{} j ! h _{N} ðQÞj v _{0} i

v

n

h j rih rj ih v _{} jC i,

ð6Þ

where we denote by jC i a superposition of eigenstates of H _{N} :

jC i ¼ ^{X} A _{v} j vi þ ^{X} ð d A ð nÞj n ^{} i,

v

n

ð7Þ

with expansion coeﬃcients A _{v} ¼ hvjh _{N} ðQÞjv _{0} i and Að nÞ¼h n ^{} jh _{N} ðQÞjv _{0} i, deter- mined by the current-triggered excitation event. The physical picture suggested by equations (6) and (7) is simple and general. The rapid electron (hole) scattering event produces a superposition of internally excited states of H _{N} . The discrete state projection of this superposition, the ﬁrst term on the right-hand side of equation (7), translates into bound-state dynamics;

Current-driven dynamics in quantum electronics

2397

vibration, rotation, intermode energy transfer or a surface exchange reaction. The scattering projection of j C i translates into bound–free dynamics, such as desorption or dissociation. Considering ﬁrst the case of bound–free dynamics, we relate the expansion coeﬃcients in equation (7) to observable probabilities by introducing a set of eigenstates j ni of an asymptotic Hamiltonian H _{N} V _{N} through

ð8Þ

j n ^{} i¼j ni þ G _{N} V _{N} j n i:

In equation (8), G _{N} is the Green operator corresponding to the Hamiltonian H _{N} and V _{N} is the potential energy operator in that Hamiltonian. In terms of the asymptotically observed states, equation (7) is written as

j C i ¼ ^{X} A _{v} jv i þ ^{X} ð d B ð n Þj n i,

v

n

ð9Þ

^{P} _{n} _{0} ^{Ð} d ^{0} h nj ^{0} n ^{0} ^{} iAð ^{0} n ^{0} Þ is the amplitude to observe the state j ni at

asymptotically long time. Formally, the B( n) are readily expressed in terms of the

scattering matrix corresponding to H _{N} . Numerically, however, it is more con- venient to solve for the nuclear dynamics in the time domain. As shown for example in [50],

where Bð nÞ ¼

jC ð t Þi ¼ ^{X} A _{v} ð t Þj vi þ ^{X} ð d A ð nt Þj n ^{} i

v

n

¼ ^{X} A _{v} ð t Þj vi þ ^{X} ð d B ð nt Þj n i,

v

n

ð10Þ

with the initial condition j C ðt ¼ 0Þi ¼ j C i: The information of interest, Bð nÞ ¼ lim _{t}_{!}_{1} ½e ^{i}^{E}^{t}^{=}^{~} Bð ntÞ ¼ lim _{t}_{!}_{1} h nj C ðtÞi, is determined by propagating the wave packet on the neutral ground surface to a long time and projecting it on to the j ni. The initial condition jC i is determined by the resonance scattering event and contains the information about the resonance state structure and lifetime. Substituting equations (6) and (9) in equation (4), we express the bound–free reaction rate as

w ð V _{b} ; Þ ¼ ð d P _{r}_{e}_{a}_{c} ð ; ÞW _{e}_{x}_{c} ð , V _{b} ; Þ,

where

P _{r}_{e}_{a}_{c} ð ; Þ ¼ ^{X} j B ð nÞj ^{2} ¼ ^{X}

n

n

lim h nj C ðt Þi

t!1

2

,

W _{e}_{x}_{c} ð , V _{b} ; Þ ¼ 2 ^{2} ^{p}

~

X

,

f _{i} ð _{} Þ½1 f _{f} ð _{} Þ jh jr i h r j ij ^{2} ð _{} _{} Þ,

ð11Þ

ð12Þ

ð13Þ

and we indicated explicitly the dependence of the rate on the bias voltage V _{b} and its parametric dependence on the resonance lifetime . Equations (11)–(13) formulate the reaction rate in terms of the current that drives the reaction; W _{e}_{x}_{c} ( , V _{b} ; ) is seen to be the resonant component of the transmission rate through the molecular junction, related to the corresponding current as W _{e}_{x}_{c} ¼ j/e, e being the electron charge. Thus, the electronic factor in equation (11), W _{e}_{x}_{c} ( , V _{b} ; ), describes the rate of excitation of the resonance, while the nuclear

2398

T. Seideman

factor, P _{r}_{e}_{a}_{c} ( ; ), is a normalized probability, describing the reaction probability per resonance excitation. Both conceptually and numerically, it is convenient to express equation (13) in terms of projected densities of states as

where

W _{e}_{x}_{c} ð , V _{b} ; Þ ¼ 2 ^{2} ^{p} ð d _{} f _{i} ð _{} Þ½1 f _{f} ð _{} Þ _{i} ð _{} Þ _{f} ð _{} Þ,

~

_{i} ð E Þ ¼ ^{X} jh jr ij ^{2} ðE _{} Þ

ð14Þ

ð15Þ

is the density of electronic states (DOS) in the initial state, projected on to the resonance orbital, and an analogous expression holds for _{f} (E). The problem of bound–bound dynamics in the nuclear modes is addressed along similar lines, the rate taking a discrete form (section 3.2). Here, however, internal relaxation needs to be taken into account, except in cases where the driving rate can be assumed fast compared with the relaxation rate.

3. Applications In this section, we describe several applications of the theory outlined in section 2. We start in section 3.1 with a discussion of scanning tunnelling microscopy (STM)-triggered reactions. In section 3.2, we turn to the problem of current-induced dynamics in single-molecule transistors.

3.1. Scanning tunnelling microscopy-triggered nanochemistry Two experimental curves of yield versus voltage are shown as symbols in ﬁgure 1. Figure 1 (a) shows the results from [51] for desorption of H atoms from H- passivated Si(100) whereas ﬁgure 1 (b) gives the data from [52] for desorption of C _{6} H _{6} from Si(100). The two reactions diﬀer substantially in detail but share several features. Both experiments [51, 52] provide evidence for an electronic mechanism; the large tip–surface distance precludes STM manipulation mechan- isms that rely on the electric ﬁeld and ﬁeld gradient at the surface or on chemical contact. The temperature dependence precludes thermal desorption. The sigmoi- dal shape of the voltage dependence in both ﬁgure 1 (a) and ﬁgure 1 (b) should be noted. These features are common also to the rate versus voltage curves of [53–55], pertaining to the rotation of DCCD on Cu(100) [53], the rotation of CCD on Cu(100) [54], and the displacement of Si adatoms on Si(111)(7 7) [55]. An interesting question in connection with ﬁgure 1 (a) is the lifetime of the underlying resonance, this problem being relevant to H-atom nanolithography with a rich variety of proven and projected applications [43–46]. Two remarkable features of ﬁgure 1 (b) are the sharp voltage dependence and the large yield observed under mild conditions; under comparable conditions rates about ﬁve orders of magnitude lower were reported for the STM-triggered resonance-mediated desorption of CO from a Cu surface [56]. The former question is addressed in section 3.1.1 and the latter in section 3.1.2. We begin this section by exploring the qualitative physics responsible for the features that are general to the STM-driven dynamics of [51–55]. To that end, we ﬁrst introduce several approximations in equation (14). Given that the tip is remote from the substrate, the coupling of the resonance to the tip continuum can

Current-driven dynamics in quantum electronics

2399

Figure 1. STM-triggered resonance-mediated desorption. (a) Desorption of H atoms from Si(100)2 1:H: (.), (m), experimental data of [51]; (—), (– – –), theoretical results of section 3.1.1. (b) Desorption of C _{6} H _{6} from Si(100): (.), experimental data of [52]; (—) theoretical results of section 3.1.2. The error bars are omitted from both sets of experimental data.

be treated as a perturbations compared with its strong interaction with the substrate continuum. Under these conditions, the projected DOSs in equation (14) can be replaced by those of the uncoupled tip and substrate–adsorbate complex. Subject to the assumption that the resonance is isolated and the DOSs of the tip and the bare substrate are almost constant on the energy scale of the resonance width, the product of DOSs in equation (14) reduces to a Lorentzian function . In the low-temperature limit the Fermi distribution functions are approximated by step functions, with which the integral over _{} is analytically soluble. One ﬁnds that

W _{e}_{x}_{c} ð , V _{b} ; Þ /

tan

tan

1

1

þ eV _{b} =2

E

F

r

E

F

r

G=2

tan

1

tan

1

E _{F} _{r} =2

E _{F} þ eV _{b} þ _{r}

G

=2

, V _{b} > 0,

, V _{b} < 0,

ð16Þ

where E _{F} is the Fermi energy, _{r} is the resonance energy and G ¼ ~= is the resonance width. The closed-form approximation of equation (16) makes explicit the physical content of the electronic function in equation (11). By contrast with an electron beam, a scanning tunnelling microscopy is a broad-band source of electrons, with an energy band of the order of e|V _{b} | . The excitation function W _{e}_{x}_{c} ( , V _{b} ; ) measures the fraction of the current that is transferred via the resonance orbital and is hence available for depositing energy into the vibrational system. Together with equation (16), equation (11) rationalizes the sigmoidal bias dependence of the rate observed experimentally [51–55]. More interestingly,

2400

T. Seideman

it suggests the possibility of extracting resonance lifetimes through ﬁt of equa- tion (11) to experimental data. This invitation is taken up in sections 3.1.1 and 3.1.2 below.

3.1.1. H-atom desorption from Si(100)2 1:H. Electron-energy-loss spectros- copy of Si(100)2 1:H showed a peak with a maximum at 8 eV and an onset at 6 eV [57]. Calculations [58] identiﬁed this feature as the ! * transition of the Si H bond, and direct optical excitation experiments with 7.9 eV light [59] conﬁrmed this assignment. The experimental results of [51] shown as full codes and full triangles in ﬁgure 1 (a) provide clear evidence for resonance-mediated desorption via the * state of the H–Si complex. Potential energy curves for motion perpendicular to the surface in the ground and the excited * states of H/Si(100) were constructed in [47] based on ab initio electronic structure calculations. These curves are used to compute the energy- resolved probability P _{r}_{e}_{a}_{c} ( , ) of equation (12) using the method discussed in [60]. Figure 2 shows the probabilities obtained as a function of the electronic-to- vibrational energy transfer and the resonance lifetime . P _{r}_{e}_{a}_{c} ( , ) is seen to be

Figure 2. Energy-resolved reaction probabilities P _{r}_{e}_{a}_{c} ð ; Þ of equation (12), for desorp- tion of H atoms from Si(100)2 1:H as a function of the scattering energy E _{B} and the resonance lifetime . (Reproduced with permission from [60].)

Current-driven dynamics in quantum electronics

2401

Figure 3. A schematic illustration of the energetics of a W-tip–Si(100):H-surface junction. Superimposed is the electronic DOS of bulk Si. The position and width of the s ! s ^{} resonance, as obtained from a ﬁt of the theoretical results to experimental data (see the text for details), are indicated by the broken curve. We note that the sample work function is 4.91 eV. (Reproduced with permission from [60].)

a narrowly distributed function of the scattering energy E _{B} (E _{B} being the

binding energy), peaked at about zero. As the lifetime increases, the distribution broadens but throughout the range of lifetimes relevant for the H/Si(100) system (vide infra) the desorbate energy distribution remains sharply peaked with width below 0.3 eV. The implications of ﬁgure 2 are discussed below. Figure 3 illustrates schematically the energetics of the W-tip–Si:H-surface junction. Since the desorption experiments [43, 45, 47, 51] considered here are performed on H-terminated surfaces, the dangling bonds, which signiﬁcantly aﬀect

the DOS of the clean Si(100) surface, do not play a role and ^{0}

is better

approximated as the density of unoccupied states of bulk Si than as that of the clean surface. This function, as computed within the density functional theory (DFT), is superimposed on the energy scheme of ﬁgure 3. Our results agree with a previous calculation of the bulk Si DOS [61]. The tip DOS is approximated as energy-independent (see [60] for a discussion of the range of validity of this approximation) and the lifetime of the Si H * state is determined by incorporating the dynamic simulation in a least-squares ﬁt loop to the data of [51]. The solid curve of ﬁgure 1 (a) gives the numerical desorption yield thus obtained. The lifetime determined is 1.2 fs, essentially independent of the substrate temperature. The H-atom desorption problem is an example of an eﬀectively one- dimensional reaction; excited-state motion is along the ground-state reaction coordinate, the transient excitation event deposits energy into the reaction mode, and intermode energy transfer does not take place. More interesting are multi- dimensional processes, where energy is initially deposited in an internal mode and is subsequently transfered to the reaction mode, owing to eﬃcient mode coupling.

The latter case is exempliﬁed by the C _{6} H _{6} /Si desorption problem, discussed in the next section.

s

3.1.2. C _{6} H _{6} desorption from Si(100). The threshold in the yield versus voltage curve of ﬁgure 1 (b) coincides to within 0.2–0.3 eV with a sharp peak in the density

2402

T. Seideman

of electronic states of C _{6} H _{6} /Si(100), indicating that a localized state is accessed in the STM-triggered tunnelling event. The peak corresponds to the binding energy of a feature observed around 2.3 eV in photoemission studies of benzene/Si(100) and attributed to the highest occupied molecular orbital of the adsorption complex [62]. These observations suggest that the desorption process summarized in ﬁgure 1 (b) is mediated by a positive-ion resonance that is predominantly localized on the adsorbate. In [52, 63] the physical considerations involved in the construction of an orthogonal coordinate system and the calculation of ab initio potential energy surfaces for the neutral and ionic states of C _{6} H _{6} /Si are discussed. Below we provide only a qualitative discussion, assisted by the contour plots of ﬁgure 4. Here Z and X are dimensionless coordinates whose mathematical deﬁnition [38] is not essential for the present discussion. In terms of physical content, Z takes the role of a desorption coordinate whereas X is a collective mode that accounts for internal

Figure 4. (a) Neutral and (b) ionic potential energy surfaces for C _{6} H _{6} /Si(100) as obtained within a cluster model at the B3LYP/6-31G** level. Superimposed on the contour plots are the conﬁgurations of the stationary states on the surfaces. (Reproduced with permission from [63].)

Current-driven dynamics in quantum electronics

2403

Figure 5. Nuclear dynamics leading to desorption of benzene molecules from a Si surface:

expectation values of X (—) and Z (– – –) in the evolving wave packet, subsequent to 25 fs evolution in the ionic state. The inset shows a snapshot of the wave packet 750 fs after relaxation, illustrating highly vibrationally mixed motion in the chemisorption well, some probability density in the physisorption site and a portion of the wave packet propagating along the exit valley. (Reproduced with permission from [64].)

motion; predominantly into-plane motion of the carbon backbone accompanied by relaxation of the Si dimer that supports the ring. The potential energy surfaces of ﬁgure 4 are employed to study the nuclear dynamics triggered by the resonance tunnelling process. Figure 5 describes the evolution in the neutral state subsequent to the resonance tunnelling event through plots of the expectation values of X and Z in the wave packet. The initial condition C is determined through 25 fs evolution in the resonant state. Desorption is initiated by large-amplitude vibrational motion across the chemisorption well. Energy initially deposited in the X mode shuttles periodically between the coupled modes for a brief period, after which the oscillation amplitude of hXi decays and desorption is under way, as indicated by a rapid increase in hZi. The inset of ﬁgure 5 shows a snapshot of the wave packet at 750 fs, illustrating vibrationally mixed motion in the chemisorption well, some probability density in a weak physisorp- tion site [63], located just beyond the transition state, and a portion of the wave packet propagating along the exit valley. With much shorter residence times (5–20 fs) in the resonance state, the tunnelling event just barely vibrationally excites the system. It undergoes low- amplitude vibrations in the well but remains bound. With much longer times in the charged state (30–40 fs) the system explores highly repulsive regions of the neutral potential energy surface, the amplitude of the short-time vibrational motion in the ring mode grows and desorption is faster [52, 64]. The time-evolving wave packet is employed to extract the energy-resolved desorption probability using the approach of [63]. As was found for the H/Si(100) system in the previous section (see ﬁgure 2), P _{r}_{e}_{a}_{c} ( ; ) for the C _{6} H _{6} /Si(100) desorption is narrowly distributed. The distribution peaks at around _{0} 1.2 eV, corresponding to a total desorbate energy _{0} E _{B} 0.3 eV. The shift from the

2404

T. Seideman

resonance energy of the threshold in the yield versus voltage curve predicted by equation (16) is thus roughly 0.3 eV, consistent with observation (ﬁgure 1 (b)). The solid curve in ﬁgure 1 (b) gives the results of a numerical ﬁt of equation (11) to the observed yield. Since our ﬁt is based on a small number of data points, and since the experimental error bars are of the order of the data, determination of a deﬁnite lifetime is not appropriate but rough upper and lower bounds can be estimated, 7 fs 9 9 17 fs: Together with ﬁgure 4, the relatively long lifetime of the adsorbate-derived C _{6} H _{6} resonance rationalizes the large yield and the sharp voltage dependence observed for this system. We remark that the ability of a two-dimensional model to capture the dynamics of the many-mode problem is due to features that are speciﬁc to the C _{6} H _{6} /Si(100) system, in particular the near conservation of C _{2}_{v} symmetry along the reaction pathway. Nonetheless, the rapid nature of the resonance-driven processes envi- saged here is expected more generally to restrict the number of active modes to relatively few. Evolution in the resonant state competes with electronic relaxation and is thus of femto second time scale. Reaction in the neutral state competes with internal relaxation and is thus of a time scale of sub- to a few picoseconds. On such short time scales, a small portion of the resonance-state potential energy surface is explored and, subsequent to electronic relaxation, energy is distributed within a restricted subset of modes.

3.2. Current-triggered dynamics in single-molecule transistors In this section, we apply the theory of section 2 to a particularly simple problem, namely current-induced vibrational excitation of a fullerene adsorbed between two Au contacts. Our choice of a simplest-case-senario model has several motivations. Firstly, an experiment by Park et al. [65] recorded the signature of current-induced vibrational motion in single Au–C _{6}_{0} –Au transistors. We are not aware of other experimental demonstrations of current-induced dynamics in a molecular device, although we believe that the concept is general ^{1} . Secondly, the Au–C _{6}_{0} –Au system oﬀers rich and relatively well-studied [66] electronic dynamics. The ability to control the electronic dynamics, already demonstrated for this system [65, 66] provides potentially a route of manipulating also the nuclear dynamics (vide infra). Thirdly, the nuclear dynamics allow for an analytical approximation which provides useful insight [66]. The molecular device in mind is depicted in ﬁgure 6. The Au electrodes extend to electron reservoirs at Z ¼ 1, where the bias voltage V _{b} is applied and electric current is collected. A metal gate with a gate voltage V _{g} is placed near the C _{6}_{0} molecule, providing a third probe capacitatively coupled to the C _{6}_{0} . In ﬁgure 7 we describe the electronic dynamics of the device of ﬁgure 6, as computed within a DFT-based non-equilibrium Green function approach [66]. The inset shows the computed transmission T(E,V _{b} ,V _{g} ) versus the electron energy E at zero bias and gate voltage. The energy scale is set such that E _{F} ¼ 0. T(E,V _{b} ,V _{g} ) is sharply peaked about E 0.15 eV, with a line shape close to the Breit–Wigner form, indicating an isolated resonance and essentially energy- independent direct transmission. This resonance is responsible for the nuclear dynamics. For reference below, we note that its width corresponds to a resonance

^{1} See Note added in proofs.

Current-driven dynamics in quantum electronics

2405

Figure 6. Current-triggered dynamics in single-molecule transistors. Schematic diagram of the Au–C _{6}_{0} –Au molecular device. The Au electrodes extend to Z ¼ 1 where the bias voltage V _{b} is applied. A gate voltage V _{g} may be applied in the scattering region of the device.

Figure 7. Electronic dynamics in the Au–C _{6}_{0} –Au device of ﬁgure 6 as obtained within a DFT-based non-equilibrium Green function approach. The main diagram shows the excitation function W _{e}_{x}_{c} of equation (14) versus the electronic-to-vibrational energy transfer and the bias voltage V _{b} . The inset gives the transmission coeﬃcient TðE,V _{b}_{,} V _{g} Þ versus energy E for zero bias and gate voltages. The transmission peak arises from the resonant orbital that mediates the current-triggered dynamics of ﬁgure 8.

lifetime of about 26 fs. At ﬁnite bias voltages V _{b} 6¼ 0, the eigenlevels, and with them the transmission peaks, shift signiﬁcantly but the overall shape of T(E,V _{b} ,V _{g} ) is only slightly modiﬁed. The eﬀect of a ﬁnite gate voltage on the transport properties is rather more substantial. By changing the charge distribution in the molecular region and shifting the energy levels, a non-zero gate voltage alters qualitatively both the line centre and the shape of the transmission curve [66]. The main diagram in ﬁgure 7 shows the excitation function W _{e}_{x}_{c} ( , V _{b} ; ) of equation (14) versus the electronic-to-vibrational energy transfer and the bias voltage V _{b} . We ﬁnd that the excitation function determined ab initio for a voltage-

2406

T. Seideman

biased molecular transistor follows nicely the form of the analytical approximation of equation (16), namely a sigmoidal function of voltage and energy. This intuitive structure is due to the near-Breit–Wigner shape of the resonance and no longer obtains in devices and energy regimes where resonances overlap. The nuclear dynamics triggered by the electronic transmission of ﬁgure 7 are similar in concept to the STM-triggered dynamics of section 3.1. The tunnelling event transiently places the nuclear system in a negative ion state of the Au–C _{6}_{0} – Au system. Owing to the equilibrium mismatch between the neutral and ionic states, a non-stationary superposition of vibrational eigenstates is formed, which travels towards the ionic state equilibrium while continuously relaxing to the neutral state. Upon electronic relaxation, the population has been redistributed between the vibrational levels of the neutral surface. This qualitative picture is quantiﬁed in ﬁgure 8. The inset shows the expecta- tion value of z in the neutral state wave packet. We ﬁnd that the C _{6}_{0} centre of mass oscillates between the contacts at the fundamental frequency of the neutral surface and an amplitude approximately equal to the distance travelled in the ionic state. Slow damping of the oscillations is due to the anharmonicity of the potential. The main diagram in ﬁgure 8 shows the vibrational excitation rate of the Au–C _{6}_{0} –Au system given by

w _{v} ðV _{b} , Þ ¼ P _{v} ð Þ W _{e}_{x}_{c} ð _{v} , V _{b} ; Þ

ð17Þ

(see equations (11) and (12)), as a function of the applied voltage V _{b} and the equilibrium displacement Z _{e}_{q} between the neutral and ion states for v ¼ 1. Our

Figure 8. Rate of vibrational excitation of the Au–C _{6}_{0} –Au device versus bias voltage (see equation (17)). The equilibrium displacement dZ _{e}_{q} between the neutral and ionic states is 1.24 pm ( f ), 4 pm (—), 10 pm ( ), 20 pm (– – –), 25 pm (— — —) and 31 pm (— –—). To allow display on the same scale, the dZ _{e}_{q} ¼ 1:24 pm results are multiplied by a factor of 5. The inset shows the expectation value of Z in the wave packet subsequent to the resonance tunnelling event.

Current-driven dynamics in quantum electronics

2407

results correspond to the unmodiﬁed molecular junction, V _{g} ¼ 0, and are given for Z _{e}_{q} values covering the physically relevant range; for smaller Z _{e}_{q} the vibrational excitation vanishes whereas for larger values we ﬁnd a ﬁnite desorption probability. The bias-voltage dependence of the w _{v} follows the V _{b} dependence of W _{e}_{x}_{c} in equation (17) (see ﬁgure 7) and is well approximated by the analytical limit of equation (16), as a result of the isolated nature of the resonance mediating the dynamics. The excitation rates of vibrational levels v > 1 take a similar shape but respond diﬀerently to the magnitude of the equilibrium displacement. We ﬁnd that the essential dynamics are contained in the combination of the equilibrium displacement and the resonance lifetime. The former parameter determines the outcome through the exponential dependence of P _{r}_{e}_{a}_{c} on Z _{e}_{q} The latter parameter determines the rate through the balance between the dependences of the electronic and nuclear dynamics. Whereas W _{e}_{x}_{c} decreases sharply with increasing (see equation (16)), P _{r}_{e}_{a}_{c} increases (roughly exponen- tially) with this parameter. The ability to manipulate the conductance by varying the distance between the electrodes and the gate voltage thereby translates into control of the current-induced dynamics.

4. Summary and outlook

In the previous sections we reviewed recent theoretical work on the problem of singe-molecule dynamics induced by electric current, a young and exciting ﬁeld that shares common aspects with several established areas of research, including transport through molecular wires, photochemistry on conducting surfaces, STM manipulation and electron–molecule scattering. Subsequent to a discussion of the qualitative physics underlying current- triggered dynamics in section 1, we outlined a theoretical framework for study of these dynamics (section 2). By introducing an approximation in the form of the electronic Hamiltonian in equation (1), we converted the solution of correlated reactions in the electronic and nuclear modes (equation (4)) into a form that provides better insight and is substantially easier to deal with numerically (equation (11)). In the latter form, the reaction rate is expressed in terms of the

resonant current j ¼ W _{e}_{x}_{c} /e that drives the reaction and a normalized reaction probability P _{r}_{e}_{a}_{c} . The parameters determining the dynamics are spelled out and the computational eﬀort is reduced to that required for a conductance calculation and a reaction dynamics calculation in the nuclear subspace. An analytical approximation of W _{e}_{x}_{c} rationalizes a common feature of several experiments, namely the sigmoidal shape of the observed rate versus voltage curves. Application was made to study STM-triggered surface reactions (section 3.1) and current- triggered dynamics in a single-molecule transistor (section 3.2). Clearly, much remains to be done in the area of current-driven dynamics in nanoscale devices. Exploring several of the potential applications proposed in section 1 is one of the topics of ongoing research in our group. In particular, we employ the concepts discussed in section 1.1 to devise a coherently driven unidirectional molecular rotor and a nanoscale rattle, to explore the modiﬁcation of the conductivity induced by current-triggered torsion in a biphenyl device (section 1.2), and to study the surface proton transfer reaction, NH _{3} /Si ! NH _{2} / SiþH/Si, mediated by a STM-triggered positive ion resonance of the substrate adsorbate complex (section 1.3).

2408

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Of considerable interest is the development of improved methods for comput- ing the electronic dynamics. Here one seeks approaches that would go beyond the current implementation of DFT, techniques that would economize the calculation and, most importantly, time-domain approaches that would provide better insight into the electronic dynamics. Another exciting avenue that we hope to address is the development of a method that goes beyond the approximation leading to equation (11) by solving simultaneously for the electronic and nuclear dynamics.

Note added in proofs In a recent conference, we became aware of an unpublished experiment by D. Ralph and coworkers, where the signature of current-driven dynamics in mol- ecular transistors was recorded.

Acknowledgments The author is grateful to several postdoctoral fellows and colleagues who contributed to the work reviewed in this article, in particular Dr Saman Alavi, Dr Roger Rousseau and Professor Hong Guo. This work was partially supported by the Natural Science and Engineering Research Council of Canada.

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