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Chemistry of Vibronic Coupling. Part 2. How to Maximize the Dynamic

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Chemistry of Vibronic Coupling. Part 2. How to Maximize the Dynamic Chemistry of vibronic coupling. Part 2. How to maximize the dynamic diagonal vibronic coupling constant forT1 states in AB systems (A, B = H, Li, Na, K, Rb, Cs, F, Cl, Br or I)?¤ Wojciech Grochala and Roald Ho†mann* Department of Chemistry and Chemical Biology, Cornell University, Ithaca, NY 18450, USA. E-mail: rh34=cornell.edu Received (in Montpellier, France) 11th May 2000, Accepted 22nd September 2000 First published as an Advance Article on the web 13th December 2000 The dynamic diagonal vibronic coupling constant (VCC) in several series of AB and AA molecules (A, B \ H, Li, Na, K, Rb, Cs, F, Cl, Br or I) has been investigated. The electronic states considered are the singlet ground state (““ionicÏÏ for heteronuclear AB species) and Ðrst excited singlet or triplet states (““covalentÏÏ). The VCC is thus studied for a charge transfer lowest lying triplet state. Qualitative trends in the VCC within the families of systems studied have been sought, with the aim of Ðnding ““a chemistry of vibronic couplingÏÏ. Two interesting correlations emerge: the VCC for the charge transfer states in an AB system grows as the sum of the electronegativities of the A and B elements increases, as well as with decreasing AB bond length. A parameter f was deÐned as the sum of the electronegativities of the A and B elements divided by the AB bond length. This leads to a nearly monotonic correlation between computed values of VCC and f for 55 molecules originating from three distinct classes with a formal single bond: intermetallic species M1M2 (M \ alkali metal), interhalogens X1X2 (X \ halogen) and salt-like compounds MX. It emerges that contracted p-type orbitals making up the r* MO (occupied by one electron in the excited state) seem to provide higher values of VCC than di†used s orbitals. The energy of the singletÈtriplet gap is also correlated with the sum of the electronegativities of the A and B elements within two families of diatomics. Quantitative explanations of these two trends are still sought. Introduction Rb, Cs, F, Cl, Br or I). In the next paper we will also look at o†-diagonal VCC for IVCT in open-shell species, such as The vibronic coupling constant (VCC, the molecular analogue 6 ““mixed valenceÏÏAB2 andB2A molecules. Subsequently we of an electronÈphonon coupling constant, EPCC, in extended aim to obtain insight into VCC in systems containing the s, p systems) is a central molecular parameter of interest in the and d block elements.7 We will try to see which kind of s, p classical BCS theory of superconductivity.2 The EPCC for an and d orbital maximizes the VCC for mixed valence tri- inter-valence (IV) charge transfer (CT) process (hereafter: atomics. Finally, we want to understand how the extension of IVCT) is believed to inÑuence the critical superconducting a molecular system into a solid a†ects the value of the VCC.8 temperature(Tc) in high-temperature cuprate and bismuthate Building a bridge between the VCC in mixed-valence cuprates superconductors.3,4 While BCS theory fails in detail for the in the solid state and the same parameter for small molecular high temperature superconductors (HTSC), there exists a systems is an important goal which is not easy to reach. monotonic relationship between values ofTc and those pre- dicted by BCS for many superconductors5 (see also Fig. 1 in ref. 6). Thus it is not surprising that in parallel with attempts Methods of calculations to formulate new theories of HTSC, e†orts continue to modify BCS theory so as to obtain better accord between theoretical The dynamic diagonal linear VCC (brieÑy referred to as the dynamic VCC, also denoted ash ) is a parameter which is and experimental results forTc . We are also interested in ee examining vibronic coupling (VC) more closely, a traditional deÐned by eqn. (1) and understandable explanatory idea of superconductivity. h \ MSe o dH/dQ o eTN at R (g) [meV A~1] (1) Our viewpoint is a chemistÏs one. We look at VCC as a ee i 0 parameter characteristic of a given molecular or extended as the average value of the derivative of energy of the state e system. Qualitative trends for the VCC in families of chemical along the ith vibration normal coordinate(Qi), calculated at systems should originate in a direct or indirect way from the the ground state (g) geometry corresponding to its (gÏs) periodic table. We try to identify such trends and to explain minimum energy,R0(g). hee is then simply the force that acts e them in as simple a way as possible. in the e state alongQi (Fi). So calculated,hee is di†erent from In the present paper we start from small molecular systems. the o†-diagonal linear VCC which describes the coupling of In this way we continue our computational investigations of electronic states g and e through the ith normal vibration and VCCs in the context of high-temperature superconductivity, is deÐned in eqn. (2). 1 begun in part 1 of this series. We examine here in detail \ ~1 values of the diagonal VCC for AB, AA and BB closed-shell heg MSg o dH/dQi o eTN at R0(g) [meV A ] (2) systems built of s- and p-block elements (A, B \ H, Li, Na, K, In the present paper we want to look only at the diagonal VCC [eqn. (1)], denoted here simply as h. The diagonal VCC ¤ For part 1, see ref. 1. is often calculated for systems with a degenerate ground state, 108 New J. Chem., 2001, 25, 108È115 DOI: 10.1039/b003779f This journal is( The Royal Society of Chemistry and the Centre National de la Recherche ScientiÐque 2001 which might be subject to a Ðrst order JahnÈTeller e†ect.9 In In most cases the ground state of a simple diatomic molecu- the Ðrst paper in our series we carefully deÐned and inter- lar species has the shortest bond length among all the elec- related the various deÐnitions of VCCs common in the liter- tronic states of the molecule. Actually, there are some ature. interesting exceptions to this rule.18 For all the systems we 10 19 We want to explore diagonal VCCs relevant to CT states. investigated theS1 states (and sometimesT1 states ) have ] Accordingly, we have chosen theS0 T1 transition, which in minima that are at longer bond lengths than that of the the heteronuclear closed-shell AB molecules we investigate is ground state. Thus, in all cases the derivatives of the energy of ] usually a r r* transition and has substantial CT character. theS1 andT1 states atR0 are negative. In this paper we ] The above is also true for theS0 S1 transition. What holds always present the absolute (positive) value of a dynamic true for the spatial part ofT1 should be roughly correct for S1 VCC. (we will probe and conÐrm this in section 1, using the LiH molecule as an example).11 Results and discussion In fact, distortion ofT1 states in diatomic molecules (towards either dissociation or just bond elongation) as The plan of this paper is as follows: in section 1 we will show studied by us in this contribution is not a textbook example of in some detail how we compute and think about the diagonal vibronic coupling. As a reviewer remarks, for such states a VCC, with the LiH molecule as an example. In section 2 we nomenclature of ““energy gradientsÏÏ instead of vibronic coup- will present computed values of the VCC for all AB molecules ling constants would suffice. However there are many connec- investigated. Finally, in section 3 we will try to summarize the tions between ““realÏÏ vibronic coupling constants and the results obtained, abstracting some simple qualitative rules for force acting at a certain nuclear arrangement in some PES. predicting values of the VCC. Our goal is to maximize the i First, the o†-diagonal vibronic coupling constantheg equals VCC within certain families of molecular species. This might the energy gradient in the most popular diabatic models of eventually provide a basis for the design of new BCS-type mixed-valence systems. Secondly, there is an important superconductors. relationship between a singletÈtriplet gap in AA diatomics and the ““realÏÏ vibronic instability of linear symmetric AAA tri- 1LiH atomics.12 Also, as we show in part 3 of this series,6 there is a connection between the force inT1 states of AB diatomics and The LiH molecule is the simplest diatomic heteronuclear mol- the vibronic stability parameter G in ABA triatomics. ecule. It has widely been investigated both in theory and experiment.20h23 In Fig. 1 we show the computed PES for the 1 \ ground state( & S0) and two lowest lying excited states Computational details 3 \ 1 \ ( & T1 and& S1) of the LiH molecule. In a one-electron To calculate the diagonal VCC for a given AB molecular picture these three states originate from a speciÐc conÐgu- system, we have scanned the potential energy surface (PES) of ration, a certain occupation of the highest occupied molecular statesg 4 S0 ande 4 T1 along the stretching normal coordi- orbital (HOMO) and the lowest unoccupied molecular orbital nate of AB molecules, using the conÐguration interaction for (LUMO) levels. TheT1 state is repulsive (dissociative), while 24 single excited states (CIS) method. The dynamic VCC was theS1 state has its minimum at about 1.9A. TheS0 ground obtained from numerical di†erentiation of the computed PES state has a certain degree of ionicity, with the LiH bond pol- ` ~ for the excitedT1 state at the ground state(S0) geometry. The arized towards H (Li H ).
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