Abstract: A method for coherent multidimensional spectroscopy may comprise illuminating a location in a sample with a set of m coherent light pulses, each coherent light pulse having an initial frequency ?m and an initial wave vector {right arrow over (k)}m, wherein m?2, to generate a coherent output signal having an initial frequency ?output=?±?m and an initial wavevector wave vector {right arrow over (k)}output=?±{right arrow over (k)}m; scanning a first coherent light pulse of the set of m coherent light pulses across a set of i frequency values, wherein i?2, the set of i frequency values including the first coherent light pulse having initial frequency ?1; scanning, simultaneously, a second coherent light pulse of the set of m coherent light pulses across a set of i correlated frequency values, the set of i correlated frequency values including the second coherent light pulse having initial frequency ?2, wherein each correlated frequency value is associated with a corresponding frequency value of the set of i frequ

Abstract: A method for coherent multidimensional spectroscopy may comprise illuminating a location in a sample with a set of m coherent light pulses, each coherent light pulse having an initial frequency ?m and an initial wave vector {right arrow over (k)}m, wherein m?2, to generate a coherent output signal having an initial frequency ?output=?±?m and an initial wavevector wave vector {right arrow over (k)}output=?±{right arrow over (k)}m; scanning a first coherent light pulse of the set of m coherent light pulses across a set of i frequency values, wherein i?2, the set of i frequency values including the first coherent light pulse having initial frequency ?1; scanning, simultaneously, a second coherent light pulse of the set of m coherent light pulses across a set of i correlated frequency values, the set of i correlated frequency values including the second coherent light pulse having initial frequency ?2, wherein each correlated frequency value is associated with a corresponding frequency value of the set of i frequ

Abstract: Methods for pump-probe spectroscopy are provided. In an embodiment, such a method comprises directing pump light having a frequency ?pump at a location in a sample to excite a transition between two quantum states of a target entity in the sample, directing probe light at the location to generate a coherent output signal having a frequency ?output and a wavevector koutput, and detecting the output signal as the probe light is scanned over a range of frequencies. In the method, either the transition excited by the pump light is a multiphoton transition corresponding to a frequency difference of n*?pump, wherein n?2; or the probe light is a set of m coherent light pulses, each coherent light pulse having a frequency ?m and a wavevector km, wherein m?2; or both. Systems for carrying out the methods are also provided.

Abstract: Methods for pump-probe spectroscopy are provided. In an embodiment, such a method comprises directing pump light having a frequency ?pump at a location in a sample to excite a transition between two quantum states of a target entity in the sample, directing probe light at the location to generate a coherent output signal having a frequency ?output and a wavevector koutput, and detecting the output signal as the probe light is scanned over a range of frequencies. In the method, either the transition excited by the pump light is a multiphoton transition corresponding to a frequency difference of n*?pump, wherein n?2; or the probe light is a set of m coherent light pulses, each coherent light pulse having a frequency ?m and a wavevector km, wherein m?2; or both. Systems for carrying out the methods are also provided.

Abstract: Methods of obtaining a multidimensional image of a sample are provided comprising (a) directing a first coherent light pulse having a first frequency ?1 and a first wave vector k1 at a first location in the sample, (b) directing a second coherent light pulse having a second frequency ?2 and a second wave vector k2 at the first location, (c) directing a third coherent light pulse having a third frequency ?3 and a third wave vector k3 at the first location and (d) detecting a coherent output signal having a fourth frequency ?4 and a fourth wave vector k4. At least two, but optionally all three, of the coherent light pulses each excite a different transition to a discrete quantum state (e.g., transitions to vibrational states or to electronic states) of a molecule or molecular functionality in the sample. Steps (a)-(d) are repeated at a sufficient number of other locations in the sample to provide the multidimensional image.

Abstract: Methods of obtaining a multidimensional image of a sample are provided comprising (a) directing a first coherent light pulse having a first frequency ?1 and a first wave vector k1 at a first location in the sample, (b) directing a second coherent light pulse having a second frequency ?2 and a second wave vector k2 at the first location, (c) directing a third coherent light pulse having a third frequency ?3 and a third wave vector k3 at the first location and (d) detecting a coherent output signal having a fourth frequency ?4 and a fourth wave vector k4. At least two, but optionally all three, of the coherent light pulses each excite a different transition to a discrete quantum state (e.g., transitions to vibrational states or to electronic states) of a molecule or molecular functionality in the sample. Steps (a)-(d) are repeated at a sufficient number of other locations in the sample to provide the multidimensional image.