Theory of nonlinear optical response of gauge invariant currents to linear and nonlinear couplings

When a gauge field interacts with a quantum condensed matter system, at first order of the gauge field it couples to the current operator of the electrons. Higher orders of the gauge field couple to electrons through other operators such as the stress tensor, etc. On the other hand, when one performs a measurement on a quantum system, not only the current operator, but also stress tensor operator of the electrons, etc. are hidden in the measurement, as they contribute to the gauge invariant current. We formulate a general problem of nonlinear optical response of the gauge invariant currents in presence of nonlinear couplings. We show that the new couplings along with new responses arising from field current have a very simple structure which can be formulated as time ordered multi-particle correlation functions. We also obtain their Lehman representation and thereby show that one need not use non-equilibrium formulations to deal with them. These new correlation functions suggest that in nonlinear optical response many new processes are possible. The experimental detection of the new terms in the current operator, and application corresponding multi-photon processes needs further theoretical and experimental investigations. (C) 2008 Elsevier B.V. All rights reserved.